耦合异质结和Pd纳米颗粒的高效电荷接力促进CO2光还原为C2H6

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中文摘要：太阳能驱动CO2转换制备高附加值产品是实现碳中和的路径之一,但具有挑战性.CO2光转化实现多碳产物的关键是打破C-C耦合难和多电子转移效率低的瓶颈.本文报道了一种由Pd修饰的BiOCl包裹CuBi2O4组成的电荷接力系统,利用PdNPs和异质结的协同作用实现CO2-C2H6的高效光转换.在无牺牲剂条件下,C2H6产率达到167.1 μmol g-1 h-1,电子选择性为81.1％.光谱研究表明,BiOCl纳米片作为电荷中继站,将光生电子从自身和CuBi2O4纳米棒定向转移到Pd纳米颗粒(PdNPs)上进行C-C耦合.PdNPs与异质结的协同作用显著提高了电荷的分离和转移效率.原位表征和理论模拟均表明,由PdNPs和异质结组成的电荷接力系统产生的富电子PdNPs,优化了CO2到C2H6反应路径,降低了中间体*CHOCO的能垒.这项工作为发展高效的CO2光催化材料提供了思路.

外文标题：Efficient charge relay steering in Pd nanoparticles coupled with the heterojunction for boosting CO2 photoreduction to C2H6

外文摘要：Solar-driven CO2 conversion to prepare value-added products is highly desirable but challenging.Central to the achievement of multi-carbon products via CO2 photo-conversion is to break the bottlenecks of C-C coupling and multi-electron transfer.Herein,a charge relay system con-sisting of Pd-decorated BiOCl-wrapped CuBi2O4 is reported by taking advantage of the synergy of Pd nanoparticles(PdNPs)and heterojunction for efficient CO2-to-C2H6 pho-toconversion.The C2H6 production rate reached 167.1 μmol g-1 h-1 with the electron selectivity of 81.1％in the absence of any sacrificial agents.The spectroscopic char-acterizations indicated that BiOCl nanosheets,acting as the charge relay,directionally transferred the photogenerated electrons from itself and CuBi2O4 nanorods to PdNPs for C-C coupling.The coordinated ensemble of PdNPs and hetero-junction significantly elevated the charge separation and transfer efficiency.Moreover,the in-situ spectroscopic analy-sis supported by theoretical simulations demonstrated that the electron-rich PdNPs generated by the charge relay of PdNPs and heterojunction optimized the CO2-to-C2H6 reaction pathway and reduced the energy barrier of the key*CHOCO intermediates.This work develops an innovative strategy to design the multifunctional catalysts for the photoconversion of CO2 to value-added carbon products.

外文关键词：

charge relayPd nanoparticlesheterojunctionCO2 photoreductionC2H6

作者：

方姣姣、朱成洋、方林灿、陈雨凯、胡慧玲、吴艳、陈庆庆、毛俊杰

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作者单位：

Key Laboratory of Functional Molecular Solids,Ministry of Education,College of Chemistry and Materials Science,Anhui Normal University,Wuhu 241002,China

Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology,Advanced Catalysis and Green Manufacturing Collaborative Innovation Center,School of Petrochemical Engineering,Changzhou University,Changzhou 213164,China

关键词：

charge relay Pd nanoparticles heterojunction CO2 photoreduction C2H6

基金：

National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaUniversity Science Research Project of Anhui ProvinceUniversity Science Research Project of Anhui Province

项目编号：

22302002223750062022AH0501822022AH020020

出版年：

2024

DOI：

10.1007/s40843-024-2995-0

中国科学:材料科学(英文)

CSTPCD

ISSN：

年,卷(期)：2024.67(9)