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作 者:Yong-Bin Chang Chao Zhang Xiu-Li Lu Wen Zhang Tong-Bu Lu
出 处:《Nano Research》2022年第1期195-201,共7页纳米研究(英文版)
基 金:supported by the National Natural Science Foundation of China(Nos.21702146,21805207,21790052,and 21931007);the National Key Technology R&D Program of China(No.2017YFA0700104);111 Project of China(No.D17003);the Natural Science Foundation of Tianjin(No.19JCQNJC05500).
摘 要:Reducing the size of heterogeneous nanocatalysts is generally conducive to improving their atomic utilization and activities in various catalytic reactions.However,this strategy has proven less effective for Cu-based electrocatalysts for the reduction of CO_(2) to multicarbon(O2+)products,owing to the overly strong binding of intermediates on small-sized(<15 nm)Cu nanoparticles(NPs).Herein,by incorporating pyreny-graphdiyne(Pyr-GDY),we successfully endowed ultrafine(〜2 nm)Cu NPs with a significantly elevated selectivity for CO_(2)-to-C_(2+)conversion.The Pyr-GDY can not only help to relax the overly strong binding between adsorbed H*and CO*intermediates on Cu NPs by tailoring the d-band center of the catalyst,but also stabilize the ultrafine Cu NPs through the high affinity between alkyne moieties and Cu NPs.The resulting Pyr-GDY-Cu composite catalyst gave a Faradic efficiency(FE)for C2+products up to 74%,significantly higher than those of support-free Cu NPs(C2+FE.〜2%),carbon nanotube-supported Cu NPs(CNT-Cu,C_(2+)FE,〜18%),graphene oxide-supported Cu NPs(GO-Cu,C_(2+)FE,〜8%),and other reported ultrafine Cu NPs.Our results demonstrate the critical influence of graphdiyne on the selectivity of Cu-catalyzed CO_(2) electroreduction,and showcase the prospect for ultrafine Cu NPs catalysts to convert CO_(2) into value-added C_(2+)products.
关 键 词:ELECTROCATALYSIS CO_(2)reduction graphdiyne nanofibers ultrafine copper nanoparticles multicarbon products
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