Poly(ethylenimine)-assisted synthesis of hollow carbon spheres comprising multi-sized Ni species for CO_(2)electroreduction

作     者：Kaining Li Yasutaka Kuwahara Hiromi Yamashita Kaining Li;Yasutaka Kuwahara;Hiromi Yamashita

作者机构：Division of Materials and Manufacturing ScienceGraduate School of EngineeringOsaka University2‐1 Yamada‐okaOsaka 565‐0871Japan Innovative Catalysis Science DivisionInstitute for Open and Transdisciplinary Research Initiatives(OTRI)Osaka University2‐1 Yamada‐okaSuitaOsaka 565‐0871Japan 

出 版 物：《Chinese Journal of Catalysis》 (催化学报（英文）)

年 卷 期：2024年第64卷第9期

页      面：66-76页

核心收录：

学科分类：081704[工学-应用化学] 07[理学] 070304[理学-物理化学(含∶化学物理)] 08[工学] 0817[工学-化学工程与技术] 0703[理学-化学] 

基　　金：Ministry of Education, Culture, Sports, Science, and Technology (MEXT) of Japan [N22H00275] Cooperative research program of "Network Joint Research Center for Materials and Devices" [20231065, 20241081] JASRI [2023B1804] China Scholarship Council 

主　　题：Hollow carbon sphere Ni nanoparticle CO_(2)reduction Electrocatalysis Single-atom catalyst 

摘      要：Electrochemical CO_(2)reduction to produce value-added chemicals and fuels is one of the research hotspots in the field of energy *** development of efficient catalysts with high conductivity and readily accessible active sites for CO_(2)electroreduction remains challenging yet *** this work,a reliable poly(ethyleneimine)(PEI)-assisted strategy is developed to prepare a hollow carbon nanocomposite comprising a single-site Ni-modified carbon shell and confined Ni nanoparticles(NPs)(denoted as Ni@NHCS),where PEI not only functions as a mediator to induce the highly dispersed growth of Ni NPs within hollow carbon spheres,but also as a nitrogen precursor to construct highly active atomically-dispersed Ni-Nx *** from the unique structural properties of Ni@NHCS,the aggregation and exposure of Ni NPs can be effectively prevented,while the accessibility of abundant catalytically active Ni-Nx sites can be *** a result,Ni@NHCS exhibits a high CO partial current density of 26.9 mA cm^(-2)and a Faradaic efficiency of 93.0%at-1.0 V ***,outperforming those of its PEI-free *** from the excellent activity and selectivity,the shell confinement effect of the hollow carbon sphere endows this catalyst with long-term *** findings here are anticipated to help understand the structure-activity relationship in Ni-based carbon catalyst systems for electrocatalytic CO_(2)***,the PEI-assisted synthetic concept is potentially applicable to the preparation of high-performance metal-based nanoconfined materials tailored for diverse energy conversion applications and beyond.