Sustainable, low-cost, high-contrast electrochromic displays via host-guest interactions.

Electrochromic (EC) displays with electronically regulating the transmittance of solar radiation offer the opportunity to increase the energy efficiency of the building and electronic products and improve the comfort and lifestyle of people. Despite the unique merit and vast application potential of EC technologies, long-awaited EC windows and related visual content displays have not been fully commercialized due to unsatisfactory production cost, durability, color, and complex fabrication processes. Here we develop a unique EC strategy and system based on the natural host and guest interactions to address the above issues. A completely reusable and sustainable EC device has been fabricated with potential advantages of extremely low cost, ideal user-/environment friendly property, and excellent optical modulation, which is benefited from the extracted biomass EC materials and reusable transparent electrodes involved in the system. The as-prepared EC window and nonemissive transparent display also show comprehensively excellent properties: high transmittance change (>85%), broad spectra modulation covering Ultraviolet (UV), Visible (Vis) to Infrared (IR) ranges, high durability (no attenuation under UV radiation for more than 1.5 mo), low open voltage (0.9 V), excellent reusability (>1,200 cycles) of the device's key components and reversibility (>4,000 cycles) with a large transmittance change, and pleasant multicolor. It is anticipated that unconventional exploration and design principles of dynamic host-guest interactions can provide unique insight into different energy-saving and sustainable optoelectronic applications.

Molecularly confined hydration in thermoresponsive hydrogels for efficient atmospheric water harvesting.

Water scarcity is a pressing global issue, requiring innovative solutions such as atmospheric water harvesting (AWH), which captures moisture from the air to provide potable water to many water-stressed areas. Thermoresponsive hydrogels, a class of temperature-sensitive polymers, demonstrate potential for AWH as matrices for hygroscopic components like salts predominantly due to their relatively energy-efficient desorption properties compared to other sorbents. However, challenges such as limited swelling capacity due to the salting-out effect and difficulty in more complete water release hinder the effectiveness of conventional hydrogel sorbents. To overcome these limitations, we introduce molecularly confined hydration in thermoresponsive hydrogels by employing a bifunctional polymeric network composed of hygroscopic zwitterionic moieties and thermoresponsive moieties. Here, we show that this approach ensures stable water uptake, enables water release at relatively low temperatures, and exhibits rapid sorption-desorption kinetics. Furthermore, by incorporating photothermal absorbers, the sorbent can achieve solar-driven AWH with comparable water release performance. This work advances the design of AWH sorbents by introducing molecularly confined hydration in thermoresponsive hydrogels, leading to a more efficient and sustainable approach to water harvesting. Our findings offer a potential solution for advanced sorbent design with comprehensive performance to mitigate the freshwater crisis.

Chemistries and materials for atmospheric water harvesting.

Atmospheric water harvesting (AWH) is recognized as a crucial strategy to address the global challenge of water scarcity by tapping into the vast reserves of atmospheric moisture for potable water supply. Within this domain, sorbents lie in the core of AWH technologies as they possess broad adaptability across a wide spectrum of humidity levels, underpinned by the cyclic sorption and desorption processes of sorbents, necessitating a multi-scale viewpoint regarding the rational material and chemical selection and design. This Invited Review delves into the essential sorption mechanisms observed across various classes of sorbent systems, emphasizing the water-sorbent interactions and the progression of water networks. A special focus is placed on the insights derived from isotherm profiles, which elucidate sorbent structures and sorption dynamics. From these foundational principles, we derive material and chemical design guidelines and identify key tuning factors from a structural-functional perspective across multiple material systems, addressing their fundamental chemistries and unique attributes. The review further navigates through system-level design considerations to optimize water production efficiency. This review aims to equip researchers in the field of AWH with a thorough understanding of the water-sorbent interactions, material design principles, and system-level considerations essential for advancing this technology.

Additives for Aqueous Zinc-Ion Batteries: Recent Progress, Mechanism Analysis, and Future Perspectives.

Aqueous zinc-ion batteries (ZIBs) stand out as a promising next-generation electrochemical energy storage technology, offering notable advantages such as high specific capacity, enhanced safety, and cost-effectiveness. However, the application of aqueous electrolytes introduces challenges: Zn dendrite formation and parasitic reactions at the anode, as well as dissolution, electrostatic interaction, and by-product formation at the cathode. In addressing these electrode-centric problems, additive engineering has emerged as an effective strategy. This review delves into the latest advancements in electrolyte additives for ZIBs, emphasizing their role in resolving the existing issues. Key focus areas include improving morphology and reducing side reactions during battery cycling using synergistic effects of modulating anode interface regulation, zinc facet control, and restructuring of hydrogen bonds and solvation sheaths. Special attention is given to the efficacy of amino acids and zwitterions due to their multifunction to improve the cycling performance of batteries concerning cycle stability and lifespan. Additionally, the recent additive advancements are studied for low-temperature and extreme weather applications meticulously. This review concludes with a holistic look at the future of additive engineering, underscoring its critical role in advancing ZIB performance amidst the complexities and challenges of electrolyte additives.

Sorbents for Atmospheric Water Harvesting: From Design Principles to Applications.

Water scarcity caused by climate change and population growth poses a grave threat to human society. Of the different water purification technologies put forward, one presents a promising strategy that is spatially or temporally non-restricted-atmospheric water harvesting (AWH). Here we review recent progress in the design and study of AWH sorbents, ranging from the innovative chemistries to the integration of sophisticated architectures and functional components, and clarify the structure-property-performance relationship that governs the water capture and release processes. Features and limitations of each type of sorbents are summarized to elucidate the optimal working environments and modes. Progress in applications extending from water generation to thermal management and agriculture are discussed. Future developments regarding material modifications, performance measurements, and system optimizations are provided to overcome lingering barriers to sorbent design and implementation.

Polyzwitterionic Hydrogels for Efficient Atmospheric Water Harvesting.

Atmospheric water harvesting (AWH) is regarded as one of the promising strategies for freshwater production desirable to provide sustainable water for landlocked and arid regions. Hygroscopic materials have attracted widespread attention because of their water harvesting performance. However, the introduction of many inorganic salts often leads to aggregation and leakage issues in practical use. Here, polyzwitterionic hydrogels are developed as an effective AWH material platform. Via anti-polyelectrolyte effects, the hygroscopic salt coordinated with polymer chains could capture moisture and enhance the swelling property, leading to a strong moisture sorption capacity. The hydrogel shows superior AWH performance (0.62 g g-1 , 120 minutes for equilibrium at 30 % relative humidity) and produces 5.87 L kg-1 freshwater per day. It is anticipated that the polyzwitterionic hydrogels with unique salt-responsive properties could provide new insights into the design and synthesis of next-generation AWH materials.

Polyzwitterionic Hydrogels for Highly Efficient High Salinity Solar Desalination.

Interfacial solar vapor generation (SVG) is regarded as a promising and sustainable strategy for clean water production. While many materials have demonstrated excellent evaporation rates under one sun, it remains challenging to design solar evaporators without compromising SVG performance in high-salinity brines (≥10 wt %). Herein, polyzwitterionic hydrogels (PZHs) are proposed as a novel platform for high-salinity solar desalination. Taking advantage of the unique anti-polyelectrolyte effects, PZHs can trap salt ions from the brine water to form a more hydrated polymer network, leading to enhanced SVG performance. PZHs exhibit an exceptional solar evaporation rate of 4.14 kg m-2 h-1 in 10 wt % brine, which is ≈20 % higher than that in pure water. It is anticipated that salt-responsive PZHs may provide insights for the design of next-generation solar desalination systems.

Carbon Materials for Solar Water Evaporation and Desalination.

Seawater desalination is viewed as a promising solution to world freshwater scarcity. Solar assisted desalination is proposed to overcome the high energy consumption in current desalination technologies, as it uses abundant and sustainable solar energy as the only energy input. Interfacial solar vapor generation (SVG) has attracted considerable research interest due to its high energy conversion efficiency, simple implementation, and cost-effectiveness. Among all the candidate materials for solar evaporators, carbon-based materials stand out due to their intrinsic high solar absorption, highly tunable structure, easy preparation, low cost, and earth-abundancy. In this review, the recent progress on carbon-based materials for the development of interfacial SVG is summarized. First, a brief introduction to the basic design principles of the interfacial SVG system is presented. Then, recent efforts in carbon-based solar evaporators, from artificial structures to bioinspired configurations, focusing on their structure-function relationship are highlighted. Strategies for designing antisalt-fouling desalination systems are also summarized. Last, the challenges and opportunities of carbon-based materials for solar evaporation technology are elaborated.

Bistable Electrochromic Ionogels via Supramolecular Interactions for Energy-Efficient Displays.

Bistable electrochromic (EC) materials and systems offer significant potential for building decarbonization through their optical modulation and energy efficiency. However, challenges such as limited design strategies and bottlenecks in cost, fabrication, and color have hindered the full commercialization of energy-saving EC windows and displays, with few materials achieving true bistability. Herein, a novel strategy for designing bistable electrochromic materials is proposed by leveraging supramolecular interactions. These interactions facilitate reversible color transitions, stabilize the colored structure, and enable spatial confinement to inhibit diffusion, thereby achieving bistable electrochromism. The mechanisms and materials underlying these unconventional electrochromic systems are substantiated through detailed characterization. This strategy enables the preparation of low-cost and sustainable transparent electrochromic displays with high performance. Notably, the display information remains clearly visible for more than 2 h without consuming energy. Involving biomass materials and removable device structures also enhances the sustainability and scalability of EC technology applications and development. These results demonstrate the crucial role of supramolecular chemistry in the development of cutting-edge materials for applications such as energy-saving smart windows.

Sustainable and Rapid Water Purification at the Confined Hydrogel Interface.

Emerging organic contaminants in water matrices have challenged ecosystems and human health safety. Persulfate-based advanced oxidation processes (PS-AOPs) have attracted much attention as they address potential water purification challenges. However, overcoming the mass transfer constraint and the catalyst's inherent site agglomeration in the heterogeneous system remains urgent. Herein, the abundant metal-anchored loading (≈6-8 g m-2) of alginate hydrogel membranes coupled with cross-flow mode as an efficient strategy for water purification applications is proposed. The organic flux of the confined hydrogel interfaces sharply enlarges with the reduction of the thickness of the boundary layer via the pressure field. The normalized property of the system displays a remarkable organic (sulfonamides) elimination rate of 4.87 × 104 mg min-1 mol-1. Furthermore, due to the fast reaction time (<1 min), cross-flow mode only reaches a meager energy cost (≈2.21 Wh m-3) under the pressure drive field. It is anticipated that this finding provides insight into the novel design with ultrafast organic removal performance and low techno-economic cost (i.e., energy operation cost, material, and reagent cost) for the field of water purification under various PS-AOPs challenging scenarios.

Hygroscopic-Microgels-Enabled Rapid Water Extraction from Arid Air.

Sorbent-based atmospheric water harvesting (AWH) has emerged as a promising decentralized water-production technology to mitigate the freshwater crisis in arid areas. Hydrogels have been regarded as attractive sorbents due to their high water retention and tailorable polymer-water interactions. Yet, the kinetics of water sorption and desorption at low relative humidity (RH) shall be improved for their practical implementation. Here, hygroscopic microgels (HMGs) composed of hydroxypropyl cellulose (HPC) and hygroscopic salt are reported, which achieve a water uptake of ca. 0.5-0.8 g g-1 at 15-30% RH. HMGs enable rapid sorption-desorption kinetics owing to the short-distance diffusion in the microgels and hydrophilicity-hydrophobicity switching of the thermoresponsive HPC. To validate the feasibility of HMGs for moisture extraction, a potential daily water collection of up to equivalent 7.9-19.1 L kg-1 at low RH is demonstrated, enabled by 24-36 operation cycles per day based on the material-level experiments. With renewable raw materials and superior performance, HMGs provide a sustainable approach for rapid moisture extraction in arid climates.

Scalable super hygroscopic polymer films for sustainable moisture harvesting in arid environments.

Extracting ubiquitous atmospheric water is a sustainable strategy to enable decentralized access to safely managed water but remains challenging due to its limited daily water output at low relative humidity (≤30% RH). Here, we report super hygroscopic polymer films (SHPFs) composed of renewable biomasses and hygroscopic salt, exhibiting high water uptake of 0.64-0.96 g g-1 at 15-30% RH. Konjac glucomannan facilitates the highly porous structures with enlarged air-polymer interfaces for active moisture capture and water vapor transport. Thermoresponsive hydroxypropyl cellulose enables phase transition at a low temperature to assist the release of collected water via hydrophobic interactions. With rapid sorption-desorption kinetics, SHPFs operate 14-24 cycles per day in arid environments, equivalent to a water yield of 5.8-13.3 L kg-1. Synthesized via a simple casting method using sustainable raw materials, SHPFs highlight the potential for low-cost and scalable atmospheric water harvesting technology to mitigate the global water crisis.

Materials Engineering for Atmospheric Water Harvesting: Progress and Perspectives.

Atmospheric water harvesting (AWH) is emerging as a promising strategy to produce fresh water from abundant airborne moisture to overcome the global clean water shortage. The ubiquitous moisture resources allow AWH to be free from geographical restrictions and potentially realize decentralized applications, making it a vital parallel or supplementary freshwater production approach to liquid water resource-based technologies. Recent advances in regulating chemical properties and micro/nanostructures of moisture-harvesting materials have demonstrated new possibilities to promote enhanced device performance and new understandings. This perspective aims to provide a timely overview on the state-of-the-art materials design and how they serve as the active components in AWH. First, the key processes of AWH, including vapor condensation, droplet nucleation, growth, and departure are outlined, and the desired material properties based on the fundamental mechanisms are discussed. Then, how tailoring materials-water interactions at the molecular level play a vital role in realizing high water uptake and low energy consumption is shown. Last, the challenges and outlook on further improving AWH from material designs and system engineering aspects are highlighted.

Tailoring the Desorption Behavior of Hygroscopic Gels for Atmospheric Water Harvesting in Arid Climates.

The ubiquitous nature of atmospheric moisture makes it a significant water resource available at any geographical location. Atmospheric water harvesting (AWH) technology, which extracts moisture from the ambient air to generate clean water, is a promising strategy to realize decentralized water production. The high water uptake by salt-based sorbents makes them attractive for AWH, especially in arid environments. However, they often have relatively high desorption heat, rendering water release an energy-intensive process. A  LiCl-incorporating polyacrylamide hydrogel (PAM-LiCl) capable of effective moisture harvesting from arid environments is proposed. The interactions between the hydrophilic hydrogel network and the captured water generate more free and weakly bonded water, significantly lowering the desorption heat compared with conventional neat salt sorbents. Benefiting from the affinity for swelling of the polymer backbones, the developed PAM-LiCl achieves a high water uptake of ≈1.1 g g-1 at 20% RH with fast sorption kinetics of ≈0.008 g g-1  min-1  and further demonstrates a daily water yield up to ≈7 g g-1 at this condition. These findings provide a new pathway for the synthesis of materials with efficient water absorption/desorption properties, to reach energy-efficient water release for AWH in arid climates.

A two-dimensional Ru@MXene catalyst for highly selective ambient electrocatalytic nitrogen reduction.

Compared with the traditional Haber-Bosch process, electrochemical ammonia synthesis has attracted much attention owing to its low energy consumption, low pollution potential, and sustainability. However, owing to the influence of high overpotential and low selectivity, the nitrogen reduction reaction (NRR) process was of limited applicability in industry. Here, we report a high-performance Ru@Ti3C2 MXene catalyst for an ambient electrocatalytic NRR. In a 0.1 M KOH electrolyte, the NH3 yield of the Ru@MXene catalyst reached 2.3 µmol h-1 cm-2, furthermore, at -0.4 V (vs. RHE) the Faraday efficiency was 13.13%.

Current Progress of Electrocatalysts for Ammonia Synthesis Through Electrochemical Nitrogen Reduction Under Ambient Conditions.

Ammonia, one of the most important chemicals and carbon-free energy carriers, is mainly produced by the traditional Haber-Bosch process operated at high pressure and temperature, which results in massive energy consumption and CO2 emissions. Alternatively, the electrocatalytic nitrogen reduction reaction to synthesize NH3 under ambient conditions using renewable energy has recently attracted significant attention. However, the competing hydrogen evolution reaction (HER) significantly reduces the faradaic efficiency and NH3 production rate. The design of high-performance electrocatalysts with the suppression of the HER for N2 reduction to NH3 under ambient conditions is a crucial consideration for the development of electrocatalytic NH3 synthesis with high FE and NH3 production rate. Five kinds of recently developed electrocatalysts classified by their chemical compositions are summarized, with particular emphasis on the relationship between their optimal electrocatalytic conditions and NH3 production performance. Conclusions and perspectives are provided for the future design of high-performance electrocatalysts for electrocatalytic NH3 production. The Review can give practical guidance for the design of effective electrocatalysts with high FE and NH3 production rates.