Janus碳壳构筑局域富质子微环境促进电催化CO2甲烷化
Janus carbon shells with inner-outer functional asymmetry enable local proton enrichment for promoting CO2 methanation
摘要
Abstract
Exploring non-copper electrocatalysts for CO2-to-CH4 electrosynthesis is important for redu-cing overreliance on copper and broadening the cata-lyst landscape.We report a strategy that enables CH4 formation on cobalt phthalocyanine(CoPc)by regu-lating the local reaction microenvironment through the catalyst structure.Ultrathin hollow carbon nano-spheres(HCNs)with a uniform size were synthes-ized and used as supports for CoPc,forming"Janus carbon shells"with inner-outer functional asym-metry.The resulting CoPc-HCN hybrid had a maxim-um CO2-to-CH4 selectivity of 15.1%,overcoming the conventional CO-selective behavior of CoPc.Mech-anistic studies show that the hollow carbon structure induces a proton enrichment outside the shell through an inner-outer surface interaction.The inner carbon surface promotes the hydrogen evolution reaction(HER)and produces a proton-enriched environment near the CoPc-active outer surface,thereby enabling CO2 methanation.This work highlights the critical role of catalyst structure in overcoming intrinsic selectivity limits of molecular catalysts.关键词
电化学 CO2 还原/甲烷/酞菁钴/Janus 碳壳/质子富集Key words
Electrochemical CO2 reduction/Methane/Cobalt phthalocyanine/Janus carbon shells/Proton enrichment引用本文复制引用
刘腾义,侯晓帆,Wijak Yospanya,叶松波,Yasutaka Matsuo,Shimpei Ono,Reiko Oda,李昊,Hiroshi Yabu..Janus碳壳构筑局域富质子微环境促进电催化CO2甲烷化[J].新型炭材料（中英文）,2026,41(3):612-625,14.基金项目
This work was supported by JSPS-KAKENHI(JP23H00301,JP24K17741,JP25K01737,JP26K 17914,and JP26K17934),JSPS Core-to-Core Program(JPJSCCA20250005),JST-MIRAI(JP-MJMI25I1),MEXT-ARIM(JPMXP1223HK 0074,JPMXP1224HK0103),the CNRS and Uni-versité de Bordeaux:the International Research Project on Chiral Field-Matter Interaction(IRP-Chi-FiMI),the IdEx Bordeaux(Research Program GPR LIGHT),the Iketani Science and Technology Founda-tion,the Hirose Foundation,the Steel Foundation for Environmental Protection Technology,and the TOKYO PRIZE Carbon Reduction.We are grateful to Mrs.Hirai and Mrs.Mori of Hokkaido University for their valuable support in HR-TEM.We gratefully ac-knowledge the Center for Computational Materials Science,Institute for Materials Research,Tohoku University for the use of MASAMUNE-IMR(202412-SCKXX-0211 and 202412-SCKXX-0209)and the Institute for Solid State Physics(ISSP)at the University of Tokyo for the use of their supercom-puters. （JP23H00301,JP24K17741,JP25K01737,JP26K 17914,and JP26K17934）
