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. 2026 Aug 20;6(9):5093–5101. doi: 10.1021/jacsau.6c00768

All-in-one Photoelectrochromic Device Enabling Designable Coloration and Real-Time Light Adaptation

Xin Guo †, Rui Zhang †, Huaihai Jin †, Ruoshi Li †, Yanan Li †, Hmbat Batelbek †, Fan Yang †, Yinglin Wang †,*, Xintong Zhang †,*, Yichun Liu †, Akira Fujishima ‡,§
PMCID: PMC13625702  PMID: 42819342

Abstract

Solar-powered electrochromic devices (SP-ECDs) are promising for zero-energy smart optical systems, holding potential applications in energy-saving windows, augmented reality displays, and adaptive camouflage. State-of-the-art SP-ECDs typically rely on the physical stacking of solar cells and electrochromic components. This approach inevitably introduces multiple heterogeneous interfaces, which severely limit the switching speed, operational stability, and color diversity of integrated devices. Herein, we introduce an all-in-one photoelectrochromic device that molecularly integrates dye-sensitized photoanodes and viologen electrochromic molecules within a single redox electrolyte. This innovative device achieves a record switching time of ∼7 s under optical, electrical, or hybrid stimuli, enabling real-time light adaptation to various dynamic illumination situations. The device presents high operational stability, enduring over 103 cycles under continuous AM 1.5G illumination. Furthermore, it offers a wide range of designable color palette (red, green, blue, purple, and cyan) with uniform, full-frame coloring appearance, facilitating further aesthetic and functional designs. Our strategy establishes a monolithic architecture that overcomes the integration complexity in conventional SP-ECDs, inspiring the creation of customized material platforms and the advancement of self-adaptive optoelectronics.

Keywords: solar-powered electrochromic, dye-sensitized solar cell, viologen, integrated device

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1. Introduction

Smart optical devices capable of autonomously responding to environmental changes hold great potential for applications in energy-saving buildings, next-generation displays, and adaptive camouflage technologies. − A key technology in this field involves electrochromic devices (ECDs), which modulate optical properties (color and transmittance) via electrical stimuli. − To enable their off-grid operation for potential portable and wearable applications, ECDs have been increasingly integrated with various energy suppliers, such as solar cells, − triboelectric nanogenerators, , and batteries. , Among these, solar-powered ECDs (SP-ECDs) stand out as particularly promising candidates, offering not only zero-energy optical modulation but also intelligent, light-responsive control. This capability greatly enhances their adaptability to dynamic lighting environments.

However, the efficient integration of solar cells with ECDs remains a major research challenge. Since Bechinger et al. first combined dye-sensitized solar cells (DSSCs) with WO3 electrochromic films via a liquid electrolyte in 1996, introducing the concept of photoelectrochromic devices (PECDs), subsequent efforts have focused on performance enhancement through structural , and compositional optimization, as well as electrolyte engineering , to improve photoelectric matching between solar-powered (SP) and electrochromic (EC) components. Recent advances have incorporated perovskite solar cells and organic photovoltaics , with electrochromic materials/devices via a multilayer stacking method, leading to a solid device architecture. Nevertheless, such stacked configurations inevitably introduce multiple solid−solid or solid–liquid interfaces, inherently leading to high interface-induced energy loss, slow switching kinetics, and limited operational stability and also restricting the material selection for wide color tunability of SP-ECDs.

To overcome these limitations, we propose an all-in-one photoelectrochromic device design that unifies solar energy conversion and electrochromic function within a homogeneous electrolyte. By dissolving viologen-based electrochromic molecules into a redox electrolyte of DSSCs, we create a multifunctional medium that simultaneously supports dye regeneration, charge transport, and electrochromic processes. This design enables direct molecular coupling between photochemical conversion and electrochromic reaction, achieving molecularly monolithic integration. As a result, we significantly broaden the compatibility between photosensitizers and electrochromic molecules, enabling multicolor outputs including red, green, blue, purple, and cyan, overcoming the monochromatic limitation of traditional devices. The resulting device exhibits a fast photoresponse of 7 s, excellent cycling stability over 1000 cycles, and stable operation under prolonged illumination exceeding 4300 s, representing a new benchmark for self-powered, adaptive optical systems.

2. Results and Discussion

2.1. All-in-One Photoelectrochromic Design

We present a monolithic, all-in-one photoelectrochromic device design achieved by incorporating viologen-based electrochromic species directly into the electrolyte of DSSCs. This design establishes an efficient molecular-level series connection between SP and EC components. As shown in Figure a and b, we utilize DSSCs as SP components, which are mainly composed of dye (D)-sensitized TiO2 mesoporous films and an electrolyte with electron mediator (Em x+). DSSCs were chosen for this work owing to their broad color palette of D molecules and high power conversion efficiency, − acting as strong candidates for building-integrated and indoor photovoltaics. To introduce the electrochromic function, we dissolve electrochromic viologen species (Es x+) at a concentration of 0.05 M into the electrolyte of DSSCs, forming the homogeneous all-in-one active medium with Em x+. Viologen species serve as the EC component, exhibiting widely tunable colors and redox potential through molecular tailoring. − These characteristics position viologens as a promising material capable of overcoming the color limitations of conventional metal oxides and polymeric EC materials. Under illumination (Figure b), photoexcited electrons generated from the D of DSSCs are injected into TiO2 and transferred to the counter electrode, driving the reduction of Es x+ species to trigger the electrochromic reaction (D + Es x+ → D+ + Es (x−1)+). Concurrently, the oxidized dye is reduced via Em x+ (D+ + Em x+ → D + Em (x+1)+), completing the dye regeneration process. In the dark, the reduced Es (x−1)+ and oxidized Em (x+1)+ in the electrolyte undergo a spontaneous homogeneous reaction, enabling rapid self-bleaching (Es (x−1)+ + Em (x+1)+ → Es x+ + Em x+). This all-in-one electrolyte integration strategy ensures the molecular-level coupling reaction between SP and EC components, fundamentally resolving the bottleneck of heterogeneous stacked architectures, such as large interfacial impedance and inefficient charge transport. Notably, Es x+ and Em x+ should exhibit matched redox potentials to enable stable and reversible redox transitions between them. The use of bare FTO (without catalyst covering) as the counter electrode of the PECD (Figure a) effectively avoids the competitive reduction reactions of both Es x+ and Em (x+1)+ at the interface of the counter electrode/electrolyte.

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All-in-one photoelectrochromic devices with various selections of materials. (a) The device structure, (b) working principle, and (c) molecule structures (D, Es x+, and Em x+) of all-in-one PECD.

2.2. Wide-Range Designable Coloration

All-in-one integration architecture fully leverages the color-mixing effects between SP and EC components, enabling broad-range color modulation with light-intensity dependence. As a representative example, we fabricated a model device denoted as Y123-Co-HV PECD, which takes Y123 as D bonding on the surface of TiO2 mesoporous films, [Co­(bpy)3]2+ redox medium (Co) as Em x+, and soluble heptyl viologen (HV) as Es x+ (all the molecular structures are shown in Figure c). The Y123 dye was selected as the primary sensitizer due to its broad light harvesting capability (350–700 nm) and high molar absorption coefficient (48,000 L mol−1 cm−1). ,, The Co redox medium serves as a high-potential redox mediator, contributing to the high photoconversion efficiency of DSSCs. , Meanwhile, the HV molecule was characterized by its low operating voltage, high coloration efficiency (180 cm2/C), and excellent stability, which represents a typical material for an all-in-one EC device.

We first optimized the thickness of Y123-sensitized photoanodes to balance the power supply and color-tuning capability of the SP unit. Although conventional high-efficiency DSSCs (PCE >14%) typically employ TiO2 mesoporous photoanodes with a thickness of around 8 μm to maximize light harvesting, such a thick photoanode exhibits an excessively deep coloration, which consequently diminishes its color-mixing effect in PECDs. To address this, we drastically reduced the thickness of the Y123-sensitized photoanode to 100 nm, which ensured the high transmittance at 460 nm of the SP unit was maintained at 61% (Figures S1 and S2). As a result, the integrated device exhibited a light-yellow appearance in the initial state (Figure a). Upon increasing the illumination intensity to 40 mW cm−2, the color of the device shifted to blue due to the formation of reduced HV+•species (absorption peak: 605 nm in Figure S3). When the thickness of the Y123-sensitized photoanode was increased to 300 and 500 nm (Figure S1), the transmittance of the photoanode was substantially reduced to 44% and 24% (at 460 nm in Figure S2), respectively. With an increased sunlight intensity to 40 mW cm−2, the Y123-Co-HV PECD (300 and 500 nm photoanodes) gradually shifted from an initial orange-red color toward purple and brown in Figure a. However, further increasing the photoanode thickness to 1 μm resulted in the photovoltaic color becoming dominant, thereby suppressing the dynamic color mixing effect of the device. The color of PECDs with different thicknesses of photoanodes exhibits a gradient deepening trend on CIE 1931 with increasing light intensity (Figure b), which is highly consistent with the optical photographs in Figure a. The corresponding transmittance spectra are shown in Figure S3.

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Wide-range designable colors of devices. (a) Appearance colors and (b) CIE 1931 color coordinates of Y123-Co-HV PECDs with different light intensities and photoanode thicknesses; (c,d) the transmittance spectra and the appearance color of all-in-one PECDs with different D and Es x+.

The molecular engineering of both SP and ECD components can be further exploited to broaden the color range of all-in-one PECDs. As illustrated in Figure c, we selected two additional viologen derivatives including a p-cyanophenyl viologen (CNV) and p-trifluoromethylphenyl viologen (CFV) in Figure c, with colored-state characteristic absorption peaks at 670 nm (green) and 540 nm (magenta), respectively (Figure S4). We then coupled them with a 100 nm-thick Y123-sensitized photoanode and Co complexes to prepare PECDs. Under illumination at 40 mW cm−2, these PECDs displayed distinctly different mixing colors: olive green and red, respectively (Figure c). When Y123 dye was replaced with the yellow L0 dye (characteristic absorption peak: 378 nm; molar absorption coefficient: 36,000 L mol−1 cm−1), combinations with these three viologen derivatives yielded PECDs that exhibited cyan-green, green, and magenta appearances under the same illumination intensity (40 mW cm−2) (Figure d). We also show the CIE 1931 color coordinates of these PECDs in Figure S5, which correspond to the optical photographs. In these all-in-one PECDs, Em x+ acts as the charge-transfer mediator between Es x+ and D, inheriting a high degree of tunability. Thereby, we configured different Em x+ such as Cu+ (Cu), , dmFc, , and TMPD , with the Y123-HV system to construct PECDs. All configured devices functioned effectively under illumination (Figure S6).

The wide color gamut in our all-in-one PECDs is attributed to efficient color mixing between SP and EC units, enabled by their homogeneous integration structure. The conventional SP-ECDs typically rely on high-efficiency SP units, such as perovskite solar cells, − DSSCs with efficient N719, , or even serial/parallel cell assemblies, to support electrochromic operation. In contrast, our all-in-one PECDs operate efficiently, driving the electrochromic switching of different viologen derivatives, even when powered only by a low-output DSSC unit with a 100 nm-thickness photoanode sensitized by Y123 or L0 dye. This low energy requirement of our all-in-one PECDs facilitates the future optimization of device structure and molecular selection for a broader color range and additional device functions. Notably, reported wide-color tunability has previously involved complex strategies such as metasurfaces or other intricate photonic structures. ,, Here, for the first time, we realize multicolor output in a simple device structure without micro/nano-structural engineering while requiring the color mixing effect among Em x+, Es x+, and D. This breakthrough not only overcomes the long-standing single-color limitation of conventional monolithic SP-ECDs but also offers a new route toward customizable coloration applications while affording substantial camouflage capability against diverse backgrounds, such as marine, forest, and desert backgrounds (Figure S7).

2.3. Fast Multi-Mode Optical Modulation

The all-in-one PECD demonstrates rapid coloration and bleaching on the scale of seconds. Under illumination at 40 mW cm−2, the Y123-Co-HV PECD achieves full coloration within 7 s. Its bleaching process is driven by a spontaneous redox reaction between Co3+ and HV+• species in the homogeneous electrolyte, enabling fast self-bleaching within 7.5 s in the dark (Figure S8). The second-scale switching performance of the all-in-one PECD is comparable to that of conventional viologen electrochromic devices ,, and significantly surpasses most monolithic solar-driven ECDs by 1 to 2 orders of magnitude , while also exceeding the switching speeds of photochromic and thermochromic technologies (Figure S9). − By combining these rapid switching speeds with the light-intensity-dependent power supply of DSSC, the all-in-one PECD exhibits outstanding light-adaptive rate under complex environmental light conditions. We systematically evaluated the optical response of the Y123-Co-HV PECD under various dynamic illumination modes, including abrupt changes (5−40 mW cm−2), continuous gradients, and random fluctuations (Figure a). The device consistently showed a coloration time of ∼7 s (purple regions) and a self-bleaching time of ∼7.5 s (green regions) across all tested light conditions. Remarkably, regardless of the modulation pathway, the device transmittance consistently stabilized at a value determined solely by the incident light intensity, as confirmed by the photographs in Figures a and S10. This reliable environmental light tracking and adaptive optical modulation allow the all-in-one PECD to perform stably under realistic dynamic conditions such as sunrise, sunset, cloud cover, or intermittent shading. Furthermore, the Y123-Co-HV PECD exhibits photothermal regulation capability, which cools the ambient temperature from 31.2 to 28.4 °C under light, heralding substantial energy savings for building air-conditioning (Figure S11). Another PECD formed by the combination of Y123-Cu-HV and Y123-TMPD-HV also reveals short light-adaptive times of 8.5/8 s and 6/6.5 s, respectively (Figure S12).

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Fast multimode optical modulation. (a) The light-adaptive ability; optical transmittance variations under (b) illumination, (c) bias, as well as (d,e) photoelectro-synergistic modulation of the Y123-Co-HV PECD.

The all-in-one architecture preserves the intrinsic operating mechanisms of both DSSC and electrochromic components, enabling not only photoelectrochromic operation driven by light but also independent electrochromic function via electrical bias. Under only illumination driving, the ΔT of the Y123-Co-HV PECD increases from 0% to ∼40% as the light intensity is raised from 0 to 20 mW cm−2 and saturates at around 40% at a higher light intensity of 40 mW cm−2 (Figure b). Instead, in the dark, the Y123-Co-HV PECD can be electrically driven with a low bias of ∼1.3 V, achieving a high ΔT of 40% (Figure c), with coloration and bleaching times of ∼7 s in Figure S13. These electrochromic performances are comparable to those achieved under illumination, establishing a foundation for performance matching in the photoelectronic synergistic operation of the device (Figure S14). For instance, the Y123-Co-HV PECD only exhibits a small ΔT of 7% under weak illumination of 5 mW cm−2, but it could immediately achieve increased ΔT of 13, 27, and 39% with the assistance of additional bias of 1.1, 1.2, and 1.3 V, respectively (Figure d). Similarly, under 1.1 V bias alone, the ΔT of Y123-Co-HV is limited to 10%, which increases to 17% with the addition of 5 mW cm−2 illumination, and is gradually elevated to 25 and 32% with the light assistance of 10 mW cm−2 and 15 mW/cm2, respectively (Figure e). These results demonstrate that all-in-one PCEDs can operate effectively under both optical and electrical stimuli and achieve synergistic enhancement of ΔT in optical–electrical hybrid mode. This optical-electrical dual-driving capability allows enhanced coloration performance in low-light conditions with minimal electrical energy input and reduced power consumption in electrical driving mode with light assistance, significantly improving the applicability and energy efficiency of all-in-one PCEDs in real-life environments.

2.4. Excellent Operational Stability

The all-in-one PECD showed exceptional operational stability (Figure S15). After 1000 light-switching cycles (illumination at 40 mW cm−2, 10 s; dark, 20 s), the device maintains nearly identical transmittance (at 605 nm) values in the colored (37%) and bleached (76%) states compared with the initial cycle (Figure a), with no observable change in coloration and bleaching time (7.5 and 7 s, respectively, in Figure b). In contrast to the conventional all-in-one viologen ECD, which requires a continuous external bias to sustain the colored state, our self-powered PECD offers a distinct advantage by reducing energy consumption by 6.5 mJ per cycle (Figure S16). Furthermore, when operating under continuous illumination (40 mW cm−2) for over 4000 s, the device exhibited negligible transmittance degradation. Even after such a long-term operation period, the device retained a rapid self-bleaching speed comparable to that of the pristine state (Figure c). This high-level stability under extreme testing conditions outperforms that of many previously reported monolithic PECDs. ,,, We attribute this high operational stability to the homogeneous, molecularly coupled architecture of all-in-one PCEDs, which facilitates the highly efficient charge-transfer pathway to reduce the risk of material photodegradation in conventional integration strategies with heterogeneous interfaces. Moreover, the PECD exhibits consistent spectral transmittance both across positions from the edge to the center and under various incident angles (Figure S17).

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Excellent operational stability. The transmittance variation at 605 nm of all-in-one PECDs during (a,b) 1000 light-switching cycles (40 mW cm−2 illumination: 10 s, dark: 20 s) and (c) continuous illumination (40 mW cm−2) over 4000 s.

3. Conclusion

In summary, we reported a novel, monolithically integrated all-in-one PECD by introducing soluble viologen electrochromic molecules into the conventional electrolyte of DSSCs. This design enables a molecular-level coupling between the photochemical solar-powered and electrochromic reactions. Our designed PECD achieves a highly integrated monolithic structure and full-frame color-tunable appearance. It achieves broad color tunability (covering red, green, blue, purple, brown, and cyan) through modulation of film thickness and component selection. It also exhibits the fastest light-adaptive response (∼7 s) compared with previously reported SP-ECDs. It demonstrates outstanding operational stability after 1000 reversible cycles and under continuous illumination of 4300 s. Our work establishes a new integration design of PECDs that overcomes the long-term limits of conventional heterogeneous-stacking integrated strategies. This study offers a facile fabrication route, extensive material selectivity, and broad applicability for the next generation of self-powered intelligent devices and encourages future research across materials science, optoelectronics, and sustainable energy technologies.

4. Experimental Section

4.1. Materials

4,4′-Bipyridine (99.7%), heptyl viologen dibromide (HV­(Br)2, 97%), lithium bis­(trifluoromethylsulfonyl)­imide (LiTFSI, 99.0%), 1,1′-dimethylferrocene (dmFc, 95%), N,N,N′,N′-tetramethyl-p-phenylenediamine (TMPD), propylene carbonate (PC, ≥99.0%), 1-butyl-3-methylimidazolium bis­(trifluoromethylsulfonyl)­imide ([BMI]­[TFSI], ≥98.0%), 2,4-dinitrochlorobenzene (≥98.0%), 4-aminobenzonitrile (≥98.0%), 4-(trifluoromethyl)­aniline (≥98.0%), 1-methylbenzimidazole (NMB, ≥99.0%), titanium tetrachloride (TiCl4, ≥99.0%), 4-(diphenylamino)­benzaldehyde (≥98.0%), methyl cyanoacetate (≥99.0%), and piperidine (≥99.5%) were purchased from Sigma-Aldrich. Y123, [Co­(bpy)3]­TFSI2, and [CuI(tmby)2]­TFSI were purchased from Dyenamo. TiO2 paste (18 NR-T) was purchased from Greatcell Solar. HV­(TFSI)2 (HV), CN-PV­(TFSI)2 (CNV), and CF3-PV­(TFSI)2 (CFV) were synthesized by using the Zincke reaction , shown in Scheme S1. And the synthesis process of L0 was also shown in Supporting Information; the detailed synthetic procedure is described in previous literature.

4.2. Preparation of the Transparent Photoanode

The TiO2 paste was diluted with anhydrous ethanol and oscillated for 0.5 h. The resulting solution was then left to stand for 2 days to obtain a TiO2 spin-coating solution with a mass fraction of 10, 20, 30, and 40 wt %.

Cleaned FTO glass substrates were treated with a 40 mM TiCl4 solution at 75 °C for 30 min. After the initial treatment, 50 μL of the TiO2 solution was spin-coated on the FTO substrate at 4000 rpm for 30 s. The sample was then placed on a hot plate at 60 °C for 5 min. Subsequently, the sample was annealed at 500 °C for 30 min to form a mesoporous TiO2 film. The obtained film was further treated with a 40 mM TiCl4 solution at 75 °C for 30 min. Afterward, the TiO2 electrode was immersed in a Y123 or L0 dye solution and soaked at room temperature for 24 h, yielding a dye-sensitized photoanode.

4.3. Fabrication of the PECDs

The photoelectrochromic electrolyte was prepared by thoroughly mixing 0.05 M Es x+, 0.05 M Em x+, and 0.6 M NMB in a solvent mixture consisting of 60 μL of PC and 50 μL of [BMI]­[TFSI]. The cleaned FTO electrode and the dye-sensitized photoanode were assembled into a sandwich-type cell structure, separated by a 60 μm-thick Surlyn film. The previously prepared photoelectrochromic electrolyte was injected into the gap between the two electrodes, and then UV-curing resin was applied to seal the edges of the device, thus completing the assembly of the PECDs.

Supplementary Material

au6c00768_si_001.pdf (2.3MB, pdf)

Acknowledgments

The work was supported by the Jilin Provincial Scientific and Technological Development Program [20250205062GH], the National Natural Science Foundation of China [62074031, 52273236, and U22A2078], and the 111 Center [B25030].

The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacsau.6c00768.

  • Synthesis of CNV, CFV, and L0; characterization of the photoanode; optical characterization and optical photographs of different PECDs; potential application; and photoelectro-synergistic mechanism (PDF)

Conceptualization: Yinglin Wang, Xintong Zhang, Yichun Liu, and Akira Fujishima. Methodology and investigation: Xin Guo, Huaihai Jin, Rui Zhang, Ruoshi Li, Yanan Li, Hmbat Batelbek, and Fan Yan. Writingoriginal draft: Xin Guo. Writingreview and editing: Yinglin Wang and Xintong Zhang.

The authors declare no competing financial interest.

Published as part of JACS Au special issue “Future Perspectives on Battery Chemistries”.

References

  1. Abraham E., Cherpak V., Senyuk B., ten Hove J.-B., Lee T., Liu Q., Smalyukh I.-I.. Highly Transparent Silanized Cellulose Aerogels for Boosting Energy Efficiency of Glazing in Buildings. Nat. Energy. 2023;8:381–396. doi: 10.1038/s41560-023-01226-7. [DOI] [Google Scholar]
  2. Barile C.-J., Slotcavage D.-J., Hou J., Strand M.-T., Hernandez T.-S., McGehee M.-D.. Dynamic Windows with Neutral Color, High Contrast, and Excellent Durability. Joule. 2017;1:133–145. doi: 10.1016/j.joule.2017.06.001. [DOI] [Google Scholar]
  3. Zhang Q., Tsai C.-Y., Li L.-J., Liaw D.-J.. Colorless-to-Colorful Switching Electrochromic Polyimides with Very High Contrast Ratio. Nat. Commun. 2019;10:1239. doi: 10.1038/s41467-019-09054-8. [DOI] [PMC free article] [PubMed] [Google Scholar]
  4. Zhang W., Li H., Yu W.-W., Elezzabi A.-Y.. Solution-Processed Vanadium Pentoxide as an Electrochromic Material for Smart Windows. Light Sci. Appl. 2020;9:121. doi: 10.1038/s41377-020-00366-9. [DOI] [PMC free article] [PubMed] [Google Scholar]
  5. Wang Z., Wang X., Cong S., Chen J., Sun H., Chen Z., Song G., Geng F., Chen Q., Zhao Z.. Tungsten Oxide@Polydopamine Core-Shell Nanowires for High-Performance Electrochromic Applications. Nat. Commun. 2020;11:302. doi: 10.1038/s41467-019-14194-y. [DOI] [PMC free article] [PubMed] [Google Scholar]
  6. Strand M.-T., Hernandez T.-S., Danner M.-G., Yeang A.-L., Jarvey N., Barile C.-J., McGehee M.-D.. Polymer Inhibitors Enable > 900 cm2 Dynamic Windows Based on Reversible Metal Electrodeposition with High Solar Modulation. Nat. Energy. 2021;6:546–554. doi: 10.1038/s41560-021-00816-7. [DOI] [Google Scholar]
  7. Kortz C., Hein A., Ciobanu M., Walder L., Oesterschulze E., Oesterschulze E.. Localized Surface Plasmon Resonance in Highly Ordered 2D Arrays of Au Nanoparticles for Electrochromic Devices. Nat. Commun. 2019;10:4874. doi: 10.1038/s41467-019-12617-4. [DOI] [PMC free article] [PubMed] [Google Scholar]
  8. Huang S., Guo H., Xia P., Sun H., Lu C., Feng Y., Zhu J., Liang C., Xu S., Wang C.. Integrated Device of Luminescent Solar Concentrators and Electrochromic Supercapacitors for Self-Powered Smart Window and Display. Nat. Commun. 2025;16:2085. doi: 10.1038/s41467-025-57369-6. [DOI] [PMC free article] [PubMed] [Google Scholar]
  9. Huang J., Ren Z., Zhang Y., Fong P.-W. K., Chandran H.-T., Liang Q., Yao K., Tang H., Xia H., Zhang H.. et al. Tandem Self-Powered Flexible Electrochromic Energy Supplier for Sustainable All-Day Operations. Adv. Energy Mater. 2022;12:2201042. doi: 10.1002/aenm.202201042. [DOI] [Google Scholar]
  10. Cho J., Yun T.-Y., Noh H.-Y., Baek S.-H., Nam M., Kim B., Moon H.-C., Ko D.-H.. Semitransparent Energy-Storing Functional Photovoltaics Monolithically Integrated with Electrochromic Supercapacitors. Adv. Funct. Mater. 2020;30:1909601. doi: 10.1002/adfm.201909601. [DOI] [Google Scholar]
  11. He Z., Gao B., Li T., Liao J., Liu B., Liu X., Wang C., Feng Z., Gu Z.. Piezoelectric-Driven Self-Powered Patterned Electrochromic Supercapacitor for Human Motion Energy Harvesting. ACS Sustain. Chem. Eng. 2019;7:1745–1752. doi: 10.1021/acssuschemeng.8b05606. [DOI] [Google Scholar]
  12. Qin S., Zhang Q., Yang X., Liu M., Sun Q., Wang Z.-L.. Hybrid Piezo/Triboelectric-Driven Self-Charging Electrochromic Supercapacitor Power Package. Adv. Energy Mater. 2018;8:1800069. doi: 10.1002/aenm.201800069. [DOI] [Google Scholar]
  13. Ma Q., Chen J., Zhang H., Su Y., Jiang Y., Dong S.. Dual-Function Self-Powered Electrochromic Batteries with Energy Storage and Display Enabled by Potential Difference. ACS Energy Lett. 2023;8:306–313. doi: 10.1021/acsenergylett.2c02346. [DOI] [Google Scholar]
  14. Zhao J., Tian Y., Wang Z., Cong S., Zhou D., Zhang Q., Yang M., Zhang W., Geng F., Zhao Z.. Trace H2O2-Assisted High-Capacity Tungsten Oxide Electrochromic Batteries with Ultrafast Charging in Seconds. Angew. Chem., Int. Ed. 2016;55:7161–7165. doi: 10.1002/anie.201602657. [DOI] [PubMed] [Google Scholar]
  15. Bechinger C., Ferrere S., Zaban A., Sprague J., Gregg B.-A.. Photoelectrochromic Windows and Displays. Nature. 1996;383:608–610. doi: 10.1038/383608a0. [DOI] [Google Scholar]
  16. Hauch A., Georg A., Krašovec U. O., Orel B.. Photovoltaically Self-Charging Battery. J. Electrochem. Soc. 2002;149:A1208–A1213. doi: 10.1149/1.1500346. [DOI] [Google Scholar]
  17. Cheng C.-Y., Chiang Y.-J., Yu H.-F., Hsiao L.-Y., Yeh C.-L., Chang L.-Y., Ho K.-C., Yeh M.-H.. Designing a Hybrid Type Photoelectrochromic Device with Dual Coloring Modes for Realizing Ultrafast Response and High Optical Contrast Self-Powered Smart Windows. Nano Energy. 2021;90:106575. doi: 10.1016/j.nanoen.2021.106575. [DOI] [Google Scholar]
  18. Krašovec U.-O., Georg A., Georg A., Wittwer V., Luther J., Topič M.. Performance of a Solid-State Photoelectrochromic Device. Sol. Energy Mater. Sol. Cells. 2004;84:369–380. doi: 10.1016/j.solmat.2004.01.043. [DOI] [Google Scholar]
  19. Wu X., Zheng J., Xu C.. Highly Optical Performance Photoelectrochromic Device Based on Br−/Br3 − Electrolyte. Electrochim. Acta. 2016;191:902–907. doi: 10.1016/j.electacta.2016.01.155. [DOI] [Google Scholar]
  20. Wu X., Zheng J., Luo G., Zhu D., Xu C.. Photoelectrochromic Devices Based on Cobalt Complex Electrolytes. RSC Adv. 2016;6:81680–81684. doi: 10.1039/C6RA17666F. [DOI] [Google Scholar]
  21. Liu Y., Wang J., Wang F., Cheng Z., Fang Y., Chang Q., Zhu J., Wang L., Wang J., Huang W.. et al. Full-Frame and High-Contrast Smart Windows from Halide-Exchanged Perovskites. Nat. Commun. 2021;12:3360. doi: 10.1038/s41467-021-23701-z. [DOI] [PMC free article] [PubMed] [Google Scholar]
  22. Zhou F., Ren Z., Zhao Y., Shen X., Wang A., Li Y.-Y., Surya C., Chai Y.. Perovskite Photovoltachromic Supercapacitor with All-Transparent Electrodes. ACS Nano. 2016;10:5900–5908. doi: 10.1021/acsnano.6b01202. [DOI] [PubMed] [Google Scholar]
  23. Yum J.-H., Baranoff E., Kessler F., Moehl T., Ahmad S., Bessho T., Marchioro A., Ghadiri E., Moser J. E., Yi C., Nazeeruddin M. K., Grätzel M.. A Cobalt Complex Redox Shuttle for Dye-Sensitized Solar Cells with High Open-Circuit Potentials. Nat. Commun. 2012;3:631. doi: 10.1038/ncomms1655. [DOI] [PMC free article] [PubMed] [Google Scholar]
  24. Higashino T., Imahori H.. Emergence of Copper­(I/II) Complexes as Third-Generation Redox Shuttles for Dye-Sensitized Solar Cells. ACS Energy Lett. 2022;7:1926–1938. doi: 10.1021/acsenergylett.2c00716. [DOI] [Google Scholar]
  25. Ren Y., Zhang D., Suo J., Cao Y., Eickemeyer F.-T., Vlachopoulos N., Zakeeruddin S.-M., Hagfeldt A., Grätzel M.. Hydroxamic Acid Pre-Adsorption Raises the Efficiency of Cosensitized Solar Cells. Nature. 2023;613:60–65. doi: 10.1038/s41586-022-05460-z. [DOI] [PubMed] [Google Scholar]
  26. Alesanco Y., Viñuales A., Cabañero G., Rodriguez J., Tena-Zaera R.. Colorless to Neutral Color Electrochromic Devices Based on Asymmetric Viologens. ACS Appl. Mater. Interfaces. 2016;8:29619–29627. doi: 10.1021/acsami.6b11321. [DOI] [PubMed] [Google Scholar]
  27. Moon H.-C., Kim C.-H., Lodge T.-P., Frisbie C.-D.. Multicolored Low-Power, Flexible Electrochromic Devices Based on Ion Gels. ACS Appl. Mater. Interfaces. 2016;8:6252–6260. doi: 10.1021/acsami.6b01307. [DOI] [PubMed] [Google Scholar]
  28. Li G., Zhang B., Wang J., Zhao H., Ma W., Xu L., Zhang W., Zhou K., Du Y., He G.. Electrochromic Poly­(Chalcogenoviologen)­s as Anode Materials for High-Performance Organic Radical Lithium-Ion Batteries. Angew. Chem., Int. Ed. 2019;58:8468–8473. doi: 10.1002/anie.201903152. [DOI] [PubMed] [Google Scholar]
  29. Pande G.-K., Choi J.-H., Lee J.-E., Kim Y.-E., Choi J.-H., Choi H.-W., Chae H.-G., Park J.-S.. Octa-Viologen Substituted Polyhedral Oligomeric Silsesquioxane Exhibiting Outstanding Electrochromic Performances. Chem. Eng. J. 2020;393:124690. doi: 10.1016/j.cej.2020.124690. [DOI] [Google Scholar]
  30. Chandrasekhar P.-S., Parashar P.-K., Swami S.-K., Dutta V., Komarala V.-K.. Enhancement of Y123 Dye-Sensitized Solar Cell Performance Using Plasmonic Gold Nanorods. Phys. Chem. Chem. Phys. 2018;20:9651–9658. doi: 10.1039/C7CP08445E. [DOI] [PubMed] [Google Scholar]
  31. Venkatesan S., Hsu T.-H., Teng H., Lee Y.-L.. Dye-Sensitized Solar Cells with Efficiency over 36% under Ambient Light Achieved by Cosensitized Tandem Structure. Sol. RRL. 2023;7:2300220. doi: 10.1002/solr.202300220. [DOI] [Google Scholar]
  32. Feldt S.-M., Wang G., Boschloo G., Hagfeldt A.. Effects of Driving Forces for Recombination and Regeneration on the Photovoltaic Performance of Dye-Sensitized Solar Cells Using Cobalt Polypyridine Redox Couples. J. Phys. Chem. C. 2011;115:21500–21507. doi: 10.1021/jp2061392. [DOI] [Google Scholar]
  33. Hao Y., Yang W., Karlsson M., Cong J., Wang S., Li X., Xu B., Hua J., Kloo L., Boschloo G.. Efficient Dye-Sensitized Solar Cells with Voltages Exceeding 1 V through Exploring Tris­(4-Alkoxyphenyl)­Amine Mediators. ACS Energy Lett. 2018;3:1929–1937. doi: 10.1021/acsenergylett.8b00872. [DOI] [Google Scholar]
  34. Guo X., Wang Y., Lin J., Li Y., Wang Y., Liu Y., Zhang X.. Electrocatalytic Anode Enabling Viologen Electrochromic Device with Low Operation Voltage below 1 V. J. Power Sources. 2024;623:235480. doi: 10.1016/j.jpowsour.2024.235480. [DOI] [Google Scholar]
  35. Ning Z., Tian H.. Triarylamine A Promising Core Unit for Efficient Photovoltaic Materials. Chem. Commun. 2009:5483–5495. doi: 10.1039/b908802d. [DOI] [PubMed] [Google Scholar]
  36. Lin J., Wang Y., Li Y., Shi Y., Guo X., Wang L., Liu Y., Zhang X.. High-Voltage Quasi-Solid-State Dye-Sensitized Solar Cells Based on Copper Redox Shuttles. Sol. RRL. 2023;7:2300464. doi: 10.1002/solr.202300464. [DOI] [Google Scholar]
  37. Tahara H., Uranaka K., Hirano M., Ikeda T., Sagara T., Murakami H.. Electrochromism of Ferrocene- and Viologen-Based Redox-Active Ionic Liquids Composite. ACS Appl. Mater. Interfaces. 2019;11:1–6. doi: 10.1021/acsami.8b16410. [DOI] [PubMed] [Google Scholar]
  38. Kim K.-W., Oh H., Bae J.-H., Kim H., Moon H.-C., Kim S.-H.. Electrostatic-Force-Assisted Dispensing Printing of Electrochromic Gels for Low-Voltage Displays. ACS Appl. Mater. Interfaces. 2017;9:18994–19000. doi: 10.1021/acsami.7b00946. [DOI] [PubMed] [Google Scholar]
  39. Ho K.-C.. The Influences of Operating Voltage and Cell Gap on the Performance of a Solution-Phase Electrochromic Device Containing HV and TMPD. Solid State Ionics. 2003;165:279–287. doi: 10.1016/j.ssi.2003.08.040. [DOI] [Google Scholar]
  40. Kao S.-Y., Kawahara Y., Nakatsuji S., Ho K.-C.. Achieving a Large Contrast, Low Driving Voltage, and High Stability Electrochromic Device with a Viologen Chromophore. J. Mater. Chem. C. 2015;3:3266–3272. doi: 10.1039/C5TC00456J. [DOI] [Google Scholar]
  41. Cannavale A., Eperon G.-E., Cossari P., Abate A., Snaith H.-J., Gigli G.. Perovskite Photovoltachromic Cells for Building Integration. Energy Environ. Sci. 2015;8:1578–1584. doi: 10.1039/C5EE00896D. [DOI] [Google Scholar]
  42. Ling H., Wu J., Su F., Tian Y., Liu Y.-J.. Automatic Light-Adjusting Electrochromic Device Powered by Perovskite Solar Cell. Nat. Commun. 2021;12:1010. doi: 10.1038/s41467-021-21086-7. [DOI] [PMC free article] [PubMed] [Google Scholar]
  43. Li C., Tao R., Ding Y., Liu C., Ding X., Xu H., Zhi C., Jia C., Li Z.. Highly Visible-Transparent and Color-Neutral Perovskite Solar Cells for Self-Powered Smart Windows. Sol. RRL. 2022;6:2101009. doi: 10.1002/solr.202101009. [DOI] [Google Scholar]
  44. Bogati S., Georg A., Graf W.. Photoelectrochromic Devices Based on Sputtered WO3 and TiO2 Films. Sol. Energy Mater. Sol. Cells. 2017;163:170–177. doi: 10.1016/j.solmat.2017.01.016. [DOI] [Google Scholar]
  45. Wu J.-J., Hsieh M.-D., Liao W.-P., Wu W.-T., Chen J.-S.. Fast-Switching Photovoltachromic Cells with Tunable Transmittance. ACS Nano. 2009;3:2297–2303. doi: 10.1021/nn900428s. [DOI] [PubMed] [Google Scholar]
  46. Xie Z., Jin X., Chen G., Xu J., Chen D., Shen G.. Integrated Smart Electrochromic Windows for Energy Saving and Storage Applications. Chem. Commun. 2014;50:608–610. doi: 10.1039/C3CC47950A. [DOI] [PubMed] [Google Scholar]
  47. Li Y., Sun P., Chen J., Zha X., Tang X., Chen Z., Zhang Y., Cong S., Geng F., Zhao Z.. Colorful Electrochromic Displays with High Visual Quality Based on Porous Metamaterials. Adv. Mater. 2023;35:2300116. doi: 10.1002/adma.202300116. [DOI] [PubMed] [Google Scholar]
  48. Xu T., Walter E.-C., Agrawal A., Bohn C., Velmurugan J., Zhu W., Lezec H.-J., Talin A.-A.. High-Contrast and Fast Electrochromic Switching Enabled by Plasmonics. Nat. Commun. 2016;7:10479. doi: 10.1038/ncomms10479. [DOI] [PMC free article] [PubMed] [Google Scholar]
  49. Sun F., Eom J.-H., Kim D.-Y., Pande G.-K., Ju H., Chae H.-G., Park J.-S.. Large-Area Flexible Electrochromic Devices with High Performance and Low-Power Consumption Enabled by Hydroxyhexyl Viologen-Substituted Polyhedral Oligomeric Silsesquioxane. ACS Sustain. Chem. Eng. 2023;11:5756–5763. doi: 10.1021/acssuschemeng.3c00381. [DOI] [Google Scholar]
  50. Chen B.-H., Kao S.-Y., Hu C.-W., Higuchi M., Ho K.-C., Liao Y.-C.. Printed Multicolor High-Contrast Electrochromic Devices. ACS Appl. Mater. Interfaces. 2015;7:25069–25076. doi: 10.1021/acsami.5b08061. [DOI] [PubMed] [Google Scholar]
  51. Meng W., Kragt A.-J. J., Gao Y., Brembilla E., Hu X., van der Burgt J.-S., Schenning A., Klein T., Zhou G., van den Ham E.-R.. et al. Scalable Photochromic Film for Solar Heat and Daylight Management. Adv. Mater. 2024;36:2304910. doi: 10.1002/adma.202304910. [DOI] [PubMed] [Google Scholar]
  52. Chen G., Wang K., Yang J., Huang J., Chen Z., Zheng J., Wang J., Yang H., Li S., Miao Y.. et al. Printable Thermochromic Hydrogel-Based Smart Window for All-Weather Building Temperature Regulation. Adv. Mater. 2023;35:2211716. doi: 10.1002/adma.202211716. [DOI] [PubMed] [Google Scholar]
  53. Liu S., Li Y., Wang Y., Du Y., Yu K. M., Yip H.-L., Jen A. K. Y., Huang B., Tso C. Y.. Mask-Inspired Moisture-Transmitting and Durable Thermochromic Perovskite Smart Windows. Nat. Commun. 2024;15:876. doi: 10.1038/s41467-024-45047-y. [DOI] [PMC free article] [PubMed] [Google Scholar]
  54. Yang S., Zheng J., Li M., Xu C.. A Novel Photoelectrochromic Device Based on Poly­(3,4-(2,2-Dimethylpropylenedioxy)­Thiophene) Thin Film and Dye-Sensitized Solar Cell. Sol. Energy Mater. Sol. Cells. 2012;97:186–190. doi: 10.1016/j.solmat.2011.09.038. [DOI] [Google Scholar]
  55. Freitag M., Gundlach L., Piotrowiak P., Galoppini E.. Fluorescence Enhancement of Di-p-Tolyl Viologen by Complexation in Cucurbit[7]­Uril. J. Am. Chem. Soc. 2012;134:3358–3366. doi: 10.1021/ja206833z. [DOI] [PubMed] [Google Scholar]
  56. Kitamura T., Ikeda M., Shigaki K., Inoue T., Anderson N.-A., Ai X., Lian T., Yanagida S.. Phenyl-Conjugated Oligoene Sensitizers for TiO2 Solar Cells. Chem. Mater. 2004;16:1806–1812. doi: 10.1021/cm0349708. [DOI] [Google Scholar]

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