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Copper compounds have been extensively investigated for diverse applications. However, studies of cuprous hydroxide (CuOH) have been scarce due to structural metastability. Herein, a facile, wet‐chemistry procedure is reported for the preparation of stable CuOH nanostructures via deliberate functionalization with select organic ligands, such as acetylene and mercapto derivatives. The resulting nanostructures are found to exhibit a nanoribbon morphology consisting of small nanocrystals embedded within a largely amorphous nanosheet‐like scaffold. The acetylene derivatives are found to anchor onto the CuOH forming CuC linkages, whereas CuS interfacial bonds are formed with the mercapto ligands. Effective electronic coupling occurs at the ligand‐core interface in the former, in contrast to mostly non‐conjugated interfacial bonds in the latter, as manifested in spectroscopic measurements and confirmed in theoretical studies based on first principles calculations. Notably, the acetylene‐capped CuOH nanostructures exhibit markedly enhanced photodynamic activity in the inhibition of bacteria growth, as compared to the mercapto‐capped counterparts due to a reduced material bandgap and effective photocatalytic generation of reactive oxygen species. Results from this study demonstrate that deliberate structural engineering with select organic ligands is an effective strategy in the stabilization and functionalization of CuOH nanostructures, a critical first step in exploring their diverse applications.

 

Vertically oriented graphene (VG) nanosheets exhibit unique structural characteristics, such as large accessible surface area, rich edges, high electrical conductivity, open network channels, and agglomeration resistance, for electrochemical energy‐storage applications (e. g., supercapacitors, lithium‐ion batteries, etc.). In this Review article, we summarize recent progress in the design and engineering of VG‐based electrodes for high‐performance electrochemical energy technologies within the context of energy‐storage mechanisms and charge‐transfer kinetics, and include a perspective to highlight the challenges and promises in the exploitation of vertically oriented two‐dimensional carbon nanostructures for further enhancement of the performance of electrochemical energy‐storage devices.

 

Developing high performance nonprecious metal‐based electrocatalysts has become a critical first step towards commercial applications of metal‐air batteries. Herein, nanocomposites based on Co/Co₂P nanoparticles encapsulated within hierarchically porous N, P, S co‐doped carbon are prepared by controlled pyrolysis of zeolitic imidazolate frameworks (ZIF‐67) and poly(cyclotriphosphazene‐co‐4,4’‐sulfonyldiphenol) (PZS). The resulting Co/Co₂P@NPSC nanocomposites exhibit apparent oxygen reduction reaction (ORR) and evolution reaction (OER) catalytic performance, and are used as the reversible oxygen catalyst for zinc‐air batteries (ZABs). Density functional theory (DFT) calculations exhibit that Co₂P could provide active sites for the ORR and promote the conversion between the adsorbed intermediates, and porous N,P,S co‐doped carbon with Co₂P nanoparticles also improves the exposure of actives sites and endows charge transport. Liquid‐state ZABs with Co/Co₂P@NPSC as the cathode catalysts demonstrate the greater power density of 198.1 mW cm⁻²and a long cycling life of 50 h at 10 mA cm⁻², likely due to the encapsulation of Co/Co₂P nanoparticles by the carbon shell. Solid‐state ZABs also display a remarkable performance with a high peak power density of 74.3 mW cm⁻². Therefore, this study indicates the meaning of the design and engineering of hierarchical porous carbon nanomaterial as electrocatalyst for rechargeable metal‐air batteries.

 

Single‐atom catalysts (SACs) have been attracting extensive interest in the electrocatalytic production of hydrogen peroxide by oxygen reduction reaction (ORR). This is due to the maximal efficiency of atom utilization and intimate interaction of the metal centers with the supporting matrix that may be exploited for deliberate manipulation of the electrocatalytic activity and selectivity, in comparison with the conventional nanoparticle counterparts. Herein, we summarize recent progress of the design and engineering of SACs towards ORR for H₂O₂generation, based on both noble and non‐noble metals. We conclude the review with a perspective highlighting the promises and challenges involved in future research.

 

Nanozymes with intrinsic enzyme-like properties and excellent stability are promising alternatives to natural enzymes. Yet, their low density of active sites and unclear crystal structure have been the major obstacles that impede their progress. Single-atom nanozymes (SAzymes) have emerged as a unique system to mitigate these issues, due to maximal atomic utilization, well-defined electronic and geometric structures, and outstanding catalytic activity distinct from their nanosized counterparts. Furthermore, the homogeneously dispersed active sites and well-defined coordination structures provide rare pathways to shed light on the catalytic mechanisms. In this review, we summarize the latest progress in the rational design and engineering of SAzymes and their applications in biomedicine and biosensing. We then conclude the review with highlights of the remaining challenges and perspectives of this emerging technology. 

Rational design and engineering of high‐performance, low‐cost electrocatalysts represents a critical first step in the development of sustainable energy technologies. While single‐atom catalysts (SACs) have emerged as viable candidates, recent research has shown that the structure and activity can be further manipulated and enhanced by the incorporation of a second metal center in the close proximity, forming a binuclear configuration. Such dual‐atom catalysts (DACs) are recognized as feasible choices to break the limitations of SACs due to the synergetic effects between the bimetallic atoms and their special structures. Herein, the recent advances of DAC electrocatalysis for a range of important reactions, focusing on their synthesis, characterization, and performance, are summarized. The review is concluded with a perspective highlighting the challenges and future research directions.