Ni single-atom sites supported on carbon aerogel for highly efficient electroreduction of carbon dioxide with industrial current densities
作者机构：State Key Laboratory of Structural ChemistryFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002China University of Chinese Academy of SciencesBeijing100049China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China FuzhouFujian350108China
出 版 物：《eScience》 (电化学与能源科学（英文）)
年 卷 期：2022年第2卷第3期
页 面：295-303页
学科分类：07[理学] 070304[理学-物理化学(含∶化学物理)] 0805[工学-材料科学与工程（可授工学、理学学位）] 0703[理学-化学]
基 金：supported by the National Key Research and Devel-opment Program of China(2018YFA0208600,2018YFA0704502) NSFC(21871263,22071245,and 22033008) Fujian Science&Technol-ogy Innovation Laboratory for Optoelectronic Information of China(2021ZZ103).
主 题：Carbon aerogel ZIF-8 Single-atom catalyst CO_(2)electrocatalysis CO
摘 要：Finding highly efficient electrocatalysts for the CO_(2)electroreduction reactions(CO_(2)RR)that have high selectivity and appreciable current density to meet commercial application standards remains a challenge.Because their reduction potentials are similar to that of the associated competitive hydrogen evolution reaction and the CO_(2)activation kinetics are sluggish.Although single-atom catalysts(SACs)with high atom efficiency are one class of promising candidates for the CO_(2)RR to produce CO,single-atom active sites supported on microporous carbons are not fully exposed to substrates and thus lead to low current density.Carbon aerogels with interconnected channels and macropores can facilitate mass transport.But few reports describe utilizing them as supports to anchor SACs for efficient electrocatalysis.Herein,N-doped carbon aerogels supporting Ni single atomic catalyst sites(denoted as Ni-NCA-X,X¼10,20)were fabricated by pyrolyzing Ni/Zn bimetallic zeolitic imidazolate framework(Ni/Zn-ZIF-8)/carboxymethylcellulose composite gels.Owing to abundant hierarchical micro-,meso-,and macropores and high CO_(2)adsorption,the Ni single active sites in the optimal Ni-NCA-10 were readily accessible for the electrolyte and CO_(2)molecules and thus achieved an industrial-level CO partial current density of 226 mA cm?2,a high CO Faradaic efficiency of 95.6%at?1.0 V vs.the reversible hydrogen electrode,and a large turnover frequency of 271810 h?1 in a flow-cell reactor at?1.0 V.Such excellent CO_(2)RR performance makes Ni-NCA-10 a rare state-of-the-art electrocatalyst for CO_(2)-to-CO conversion.This work provides an effective strategy for designing highly efficient electrocatalysts toward the CO_(2)RR to achieve industrial current density via anchoring single-atom sites on carbon aerogels.
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