Anodic Electrosynthesis of Amide from Alcohol and Ammonia

Amide is essential in biologically active compounds,synthetic materials,and building blocks.However,conventional amide production relies on energyintensive consumption and activating agents that modulate processes to construct the C–N bond.Herein,for the first time,we have successfully realized the formation of amides at industrial current density via the anodic coelectrolysis of alcohol and ammonia under ambient conditions.We have proved thatmodulation of the interface microenvironment concentration of nucleophile by electrolyte engineering can regulate the reaction pathways of amides rather than acetic acids.The C-N coupling strategy can be further extended to the electrosynthesis of the long-chain and aryl-ring amide with high selectivity by replacing ammonia with amine.Our work opens up a vast store of information on the utilization of biomass alcohol for high-value N-containing chemicals via an electrocatalytic C-N coupling reaction.

Doping-driven dual heterogeneous interfacial structures boosting the durability of industry-compatible water splitting at high current density

Developing highly stable electrocatalysts under industry-compatible current densities(>500 mA cm^(-2))in an anion-exchange membrane water electrolyzer(AEMWE)is an enormous challenge for water splitting.Herein,based on the results of density function theory calculations,a dual heterogeneous interfacial structured NiSe/Fe-Ni(OH)_(2)catalyst was subtly designed and successfully prepared by electrodepositing Fe-doped Ni(OH)_(2)on NiSe-loaded nickel foam(NF).Fe doping-driven heterogeneous structures in NiSe/Fe-Ni(OH)_(2)markedly boost catalytic activity and durability at industrially compatible current densities in single hydrogen and oxygen evolution reactions under alkaline conditions.In particular,NiSe/Fe-Ni(OH)_(2)shows a negligible performance loss at 600 mA cm^(-2)at least 1,000 h for overall water splitting,a distinguished long-term durability acting as AEMWE electrodes at 600 mA cm^(-2)and 1 A cm^(-2)at 85℃for at least 95 h.Owing to Fe doping-induced strong synergetic effect between Ni and Fe,dual heterostructure-promoted charge transfer and redistribution,abundant catalytic active sites,and improvement of stability and durability,a mechanism of Fe doping-driven heterogeneous interfacial structurepromoted catalytic performance was proposed.This study provides a successful example of theory-directed catalyst preparation and pioneers a creative strategy for industry-compatible water splitting at high current density.

Defect spinel oxides for electrocatalytic reduction reactions

Electrocatalytic reduction reactions play a crucial role in electrochemical energy conversion and storage technology,which are emerging technologies to ameliorate environmental problems.Spinel oxides are widely explored in electrocatalytic oxidation reactions but have a poor intrinsic ability to reduction reactions,making their electrocatalytic ability less effective.To improve this,defect engineering is a valuable method for regulating the electronic structure and coordination environment.Herein,this manuscript discusses the use of defect spinel oxides in electrocatalytic reduction reactions,including the different types of defects,construction methods,and characterization techniques.It also outlines the various applications of defect spinel oxides in different electrocatalytic reduction reactions.Finally,it goes over the challenges and future outlooks for defect spinels.This review aims to thoroughly explain how defect spinels work in electrocatalytic reduction reactions and serve as a helpful guide for creating effective electrocatalysts.

缺陷g-C_(3)N_(4)优化催化层的磷酸分布以提高高温质子膜燃料电池的性能

磷酸作为质子传导介质对于高温质子膜燃料电池是至关重要的但调节磷酸分布来减少电催化剂中毒及保持高反应性的稳定性仍面临挑战.在本工作中,缺陷g-C_(3)N_(4)被分散到Pt/C催化层中促进磷酸的分布来提高催化剂的本征活性表达.由于缺陷g-C_(3)N_(4)修饰,低铂负载量在阳极(0.20 mgPtcm^(-2))和阴极(0.40 mgPtcm^(-2))条件下,高温质子膜燃料电池呈现一个高的峰功率672 mW cm^(-2)和高反应性(高于620 mW cm^(-2)),且具有3500个加速循环的优越稳定性,该性能优于目前报道的结果.本工作首次揭示了缺陷g-C_(3)N_(4)与磷酸的酸碱相互作用可调节催化层的磷酸分布,从而提高催化剂的本征活性表达和利用率.