A quartet dual-band electrochromic device (ECD) was developed to selectively control the transmittance from the visible to near-infrared wavelengths for the application of an energy-efficient smart window. The new AgNO3+TBABr+LiClO4 (ATL)-based electrolyte was developed to independently control the redox reaction of lithium and silver ions to demonstrate the quartet mode of an ECD. A dual-band ECD with a sandwich structure was assembled using an ATL-based electrolyte, WO3 electrochromic layer, and antimony-doped tin oxide (ATO) ion storage layer. The employed WO3 and ATO films were fabricated using a nanoparticle deposition system (NPDS), a novel ecofriendly dry deposition method. Four modes, namely, transparent, warm, cool, and all-block modes, were demonstrated via an independent redox reaction of both lithium and silver ions through the simple control of the applied voltage. In the warm mode, the localized surface plasmon resonance effect was exploited by producing silver nanoparticles upon two-step voltage application. Furthermore, since the high surface roughness of the WO3 thin film fabricated by NPDS maximized the light scattering effect, 0% transmittance at all wavelengths was observed in the all-block mode. Dual-band ECD showed high optical contrasts of 73% and long-term durability over 1000 cycles with no degradation. Therefore, the possibility of controlling transmittance at the target wavelength was confirmed using a simple device with a simple process, suggesting a new strategy for the design of dual-band smart windows to reduce the energy consumption of buildings.

High Optical Contrast of Quartet Dual-Band Electrochromic Device for Energy-Efficient Smart Window.

Electrochromic devices (ECDs) show promising applications in various fields including energy‐saving smart windows, energy‐recycling batteries/supercapacitors, displays, thermal management, etc. Compared to monovalent cations (H+, Li+, Na+, and K+), multivalent‐ion carriers (Mg2+, Ca2+, Zn2+, and Al3+) can enable the ECDs with high optical contrast, high energy‐recycling capability, and attractive long‐term stability because of the multiple‐electron transfer redox. Additionally, Mg2+, Zn2+, and Al3+‐based ECDs assembled with metal anodes are exploited for applications in EC electronics, EC mirrors, flexible devices, etc. Attempts to develop multivalent‐ion ECDs can be traced to 2013. However, since 2017, the research activity in this field has surged in the world. Despite the fascinating achievements, there is still a long way from their maturity due to challenges related to the limited electrode materials and electrolytes, as well as the obscure multivalent‐ion redox mechanisms. This review aims to discuss 1) the EC mechanisms of electrode materials with multivalent ions, 2) the advantageous functionalities of multivalent‐ion ECDs, and 3) strategies developed for exploring electrode materials, electrolytes, and ECD structures. Additionally, future perspectives for remaining challenges and corresponding strategies for developing multivalent‐ion ECDs with designed functionalities are discussed.

Multivalent‐Ion Electrochromic Energy Saving and Storage Devices

Electrochromic technology has witnessed numerous achievements in recent years both in research and commercialization. Electrochromic devices (ECD) based on different electrochemical mechanism have been developed for various applications, ranging from smart windows, thermal management, rear views, display, camouflage, etc. Compared to conventional ECDs based on monovalent charge carriers (e.g., H+, Li+), incorporating multivalent ions with rich electrochemistry, high charge density, and small ionic radius has opened new possibilities in novel ECDs. The merits of multivalent ions are harvested in ECDs activated by ion intercalation/deintercalation (e.g., Zn2+, Al3+, Ca2+, Mg2+), reversible metal electrodeposition (e.g., Cu2+, Bi3+, Zn2+), and dynamic metal–ligand interactions (e.g., Cu2+, Fe2+). Herein, the working mechanism, characteristics, and up‐to‐date achievements in multivalent ECDs are summarized and classified accordingly. The applications of multivalent ECDs for smart windows, energy storage, thermal management, multicolor displays, etc., are exemplified. The issues and challenges encountered by multivalent ECDs are emphasized, and the future directions for developing multivalent ECDs are also summarized. The aim of this review is to inspire more efforts in the exploration and the proliferation of multivalent ECDs.

The Progress and Outlook of Multivalent‐Ion‐Based Electrochromism

Isomeric effects of poly-viologens on electrochromic performance and applications in low-power electrochemical devices

Electrochromic technology offers exciting opportunities for smart applications such as energy-saving and interactive systems. However, achieving dual-band regulation together with the multicolor function is still an unmet challenge for electrochromic devices. Herein, an ingenious electrochromic strategy based on reversible manganese oxide (MnO2 ) electrodeposition, different from traditional ion intercalation/deintercalation-type electrochromic materials is proposed. Such a deposition/dissolution-based MnO2 brings an intriguing electrochromic feature of dual-band regulation for the ultraviolet (UV) and visible lights with high optical modulation (93.2% and 93.6% at 400 and 550 nm, respectively) and remarkable optical memory. Moreover, a demonstrative smart window assembled by MnO2 and Cu electrodes delivers the electrochromic properties of effective dual-band regulation accompanied by multicolor changes (transparent, yellow, and brown). The robust redox deposition/dissolution process endows the MnO2 -based electrochromic device with excellent rate capability and an areal capacity of 570 mAh m-2 at 0.1 mA cm-2 . It is believed that the metal oxide-based reversible electrodeposition strategy would be an attractive and promising electrochromic technology and provide a train of thought for the development of multifunctional electrochromic devices and applications.

A Reversible MnO2 Deposition-Enabled Multicolor Electrochromic Device with Efficient Tunability of Ultraviolet-Visible Light.

Multicolor Electrochromic Device based on Reversible Metal Electrodeposition of Bi-Cu with Controlled Morphology and Composition Ratio

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Multicolor Electrochromic Device based on Reversible Metal Electrodeposition of Bi-Cu with Controlled Morphology and Composition Ratio

Five-State Flexible Dynamic Windows