Electrochemical reduction of CO2 to obtain high-value-added feedstocks is a promising strategy to alleviate the energy crisis. Cu-based catalysts generate multi-carbon products with high activity in the CO2 reduction reaction (CO2RR), although great challenges remain in the selectivity and stability of Cu-based catalysts. Here, highly active Cu/Cu2O nanoclusters were produced via in situ electrochemical reconstruction using Cu–N coordinated MOFs as precursors for the highly selective C2H4 synthesis, showing a Faradaic efficiency of 70.2 ± 1.7% toward C2H4 with a partial current density of 12.38 mA·cm–2 at −1.03 V vs RHE in the CO2RR. In situ infrared spectroscopy with the observation of *CO*CO and *CO*COH intermediates confirmed the C2H4 formation pathway, while in situ Raman spectroscopy, ex situ XPS, and HRTEM evidenced that the coexisting Cu2O and Cu nanoclusters were the active sites. The in situ reconstruction method could be used to synthesize catalysts with high activity and selectivity for CO2 electroreduction. 

In Situ Reconstruction of Cu–N Coordinated MOFs to Generate Dispersive Cu/Cu2O Nanoclusters for Selective Electroreduction of CO2 to C2H4

Abstract Achieving a highly robust zinc (Zn) metal anode is extremely important for improving the performance of aqueous Zn-ion batteries (AZIBs) for advancing “carbon neutrality” society, which is hampered by the uncontrollable growth of Zn dendrite and severe side reactions including hydrogen evolution reaction, corrosion, and passivation, etc. Herein, an interlayer containing fluorinated zincophilic covalent organic framework with sulfonic acid groups (COF-S-F) is developed on Zn metal (Zn@COF-S-F) as the artificial solid electrolyte interface (SEI). Sulfonic acid group (− SO 3 H) in COF-S-F can effectively ameliorate the desolvation process of hydrated Zn ions, and the three-dimensional channel with fluoride group (-F) can provide interconnected channels for the favorable transport of Zn ions with ion-confinement effects, endowing Zn@COF-S-F with dendrite-free morphology and suppressed side reactions. Consequently, Zn@COF-S-F symmetric cell can stably cycle for 1,000 h with low average hysteresis voltage (50.5 mV) at the current density of 1.5 mA cm −2 . Zn@COF-S-F|MnO 2 cell delivers the discharge specific capacity of 206.8 mAh g −1 at the current density of 1.2 A g −1 after 800 cycles with high-capacity retention (87.9%). Enlightening, building artificial SEI on metallic Zn surface with targeted design has been proved as the effective strategy to foster the practical application of high-performance AZIBs. 

Covalent Organic Framework with 3D Ordered Channel and Multi-Functional Groups Endows Zn Anode with Superior Stability

Coupling photocatalytic H2 evolution with benzyl alcohol (BA) oxidation to benzaldehyde (BAD) reaction allows the full utilization of the energy of light-induced electron and hole to produce fuel and valuable chemicals, which has received widespread attention recently. Herein, Co(OH)2 nanosheet array-graphene(GR) composites cocatalyst can be successfully synthesized by simple precipitation method, and then CdS nanoparticles are in situ grown in hybrid cocatalyst to finally obtain CdS-Co(OH)2-GR ternary photocatalysts. Composting of dual-cocatalyst with CdS facilitates the migration of photoinduced charge carriers of CdS, affords abundant active sites and makes the growth of CdS nanoparticles more uniform and dispersed. As a result, the CdS-Co(OH)2-GR ternary composites have shown a glorious performance, showing the H2 generation velocity of 1173.53 µmol h−1 g−1, and the conversion rate of benzyl alcohol has reached 100 % within 2 h, which has surpassed other prepared samples and most of analogous photocatalyst systems. We are confident that this study can supply a useful reference for the synthesis of dual-cocatalyst-modified semiconductor composites, and promote the development of photocatalytic coupling reaction system, in which sacrifice agents are free and energies of light-induced electron and holes can be fully utilized. 

Decorating CdS with cobaltous hydroxide and graphene dual cocatalyst for photocatalytic hydrogen production coupled selective benzyl alcohol oxidation

Rechargeable batteries, typically represented by lithium-ion batteries, have taken a huge leap in energy density over the last two decades. However, they still face material/chemical challenges in ensuring safety and long service life at temperatures beyond the optimum range, primarily due to the chemical/electrochemical instabilities of conventional liquid electrolytes against aggressive electrode reactions and temperature variation. In this regard, a gel polymer electrolyte (GPE) with its liquid components immobilized and stabilized by a solid matrix, capable of retaining almost all the advantageous natures of the liquid electrolytes and circumventing the interfacial issues that exist in the all-solid-state electrolytes, is of great significance to realize rechargeable batteries with extended working temperature range. We begin this review with the main challenges faced in the development of GPEs, based on extensive literature research and our practical experience. Then, a significant section is dedicated to the requirements and design principles of GPEs for wide-temperature applications, with special attention paid to the feasibility, cost, and environmental impact. Next, the research progress of GPEs is thoroughly reviewed according to the strategies applied. In the end, we outline some prospects of GPEs related to innovations in material sciences, advanced characterizations, artificial intelligence, and environmental impact analysis, hoping to spark new research activities that ultimately bring us a step closer to realizing wide-temperature rechargeable batteries.

Gel polymer electrolytes for rechargeable batteries toward wide-temperature applications.

To cater to the swift advance of flexible wearable electronics, there is growing demand for flexible energy storage system (ESS). Aqueous zinc ion energy storage systems (AZIESSs), characterizing safety and low cost, are competitive candidates for flexible energy storage. Hydrogels, as quasi-solid substances, are the appropriate and burgeoning electrolytes that enable high-performance flexible AZIESSs. However, challenges still remain in designing suitable and comprehensive hydrogel electrolyte, which provides flexible AZIESSs with high reversibility and versatility. Hence, the application of hydrogel electrolyte-based AZIESSs in wearable electronics is restricted. A thorough review is required for hydrogel electrolyte design to pave the way for high-performance flexible AZIESSs. This review delves into the engineering of desirable hydrogel electrolytes for flexible AZIESSs from the perspective of electrolyte designers. Detailed descriptions of hydrogel electrolytes in basic characteristics, Zn anode, and cathode stabilization effects as well as their functional properties are provided. Moreover, the application of hydrogel electrolyte-based flexible AZIESSs in wearable electronics is discussed, expecting to accelerate their strides toward lives. Finally, the corresponding challenges and future development trends are also presented, with the hope of inspiring readers. 

Hydrogel Electrolyte Enabled High-Performance Flexible Aqueous Zinc Ion Energy Storage Systems toward Wearable Electronics.

A hydrogel electrolyte with ultrahigh ionic conductivity and transference number benefit from Zn2+ “highways” for dendrite-free Zn-MnO2 battery

In response to the growing demand for wearable devices and environmental monitoring, this study presents a novel fabrication method for directionally aligned CNFs/MWCNTs aerogel film (AGF), thereby achieving high-performance, flexible humidity sensors with rapid response and excellent mechanical properties. By combining freeze-drying and directional freezing techniques, an ordered porous structure within the AGF was created to promote efficient water molecule exchange and optimized conductivity. The sensor sensitivity was fine-tuned by adjusting the MWCNTs content, reaching a peak response of 71.5% (ΔI/I0) at 75% RH, with response and recovery times of 18 s and 47 s, respectively. This surpasses the performance of traditional sensors based on CNFs/MWCNTs. Upon evaluating the mechanical properties of AGF, it was found that they possessed outstanding flexibility and bending resistance, making them highly suitable for wearable electronic applications. The versatility of AGF sensors was demonstrated in various humidity monitoring scenarios, such as close-range positioning of moist objects and real-time human breathing monitoring. To showcase practical applicability, an STM32-based smart wireless humidity monitoring system suitable for real-time data collection, remote monitoring, and flexible installation was developed. Moreover, this fabrication method holds vast potential in various application fields, including wearable devices, environmental monitoring, and electronic skin. 

A CNFs/MWCNTs aerogel film-based humidity sensor with directionally aligned porous structure for substantially enhancing both sensitivity and response speed

Urea perylene imide polymer (UPDI) is successfully recombined with Co(NO3)2 molecules into one-dimensional nanocrystals (Co−UPDI) for enhanced photocatalytic oxygen evolution (POE) under visible light. Co−UPDI as photocatalyst exhibits more an order of magnitude of POE rate than UPDI at pH = 4.8 (8.00 vs. 0.58 mmol h−1g−1), which is the highest among reported POE tests in aqueous colloid system with AgNO3 as sacrificial agent. The apparent quantum yield (AQY) reaches 4.39 % at 450 nm. The systematical experiments reveals that the heterojunction formation between UPDI line and Co(NO3)2 molecules is crucial through the coordination of Co with N atoms. Consequently, the rigidity of UPDI line enhances, H−type stacking of PDI moiety becomes closer, and CoOOH as cocatalyst in-situ forms during POE. Meanwhile, more excitons with longer lifetime generate and more quickly transfer in Co−UPDI than UPDI nanocrystals. This work provides an efficient strategy for photocatalytic water oxidation. 

Cobalt-intercalated One-dimensional Nanocrystals of Urea Perylene Imide Polymer for Enhanced Visible-light Photocatalytic Water Oxidation

Electrocatalytic reduction of CO2 with non-precious materials containing Co-N-C moiety as catalyst is considered to be a promising method for carbon neutrality. Unfortunately, metal phthalocyanine with an intrinsic Co–pyrrolic N4–C...

Controllable dispersion of cobalt phthalocyanine molecules on graphene oxide for enhanced electrocatalytic reduction of CO2 to CO

Morphology-dependent Photoelectric Properties and Photocatalytic CO2 Reduction of Zinc Porphyrin Nanocrystals

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