Boosting CO2 Electroreduction to C2H4 via Unconventional Hybridization: High-Order Ce4+ 4f and O 2p Interaction in Ce-Cu2O for Stabilizing Cu+

Boosting(机器学习) 材料科学 订单(交换) 物理 计算机科学 机器学习 财务 经济
作者
Yanfei Sun,Jiangzhou Xie,Zhenzhen Fu,Huiying Zhang,Yebo Yao,Yixiang Zhou,Xiaoxuan Wang,Shiyu Wang,Xueying Gao,Zheng Tang,Shuyuan Li,Xiaojun Wang,Kaiqi Nie,Zhiyu Yang,Yi‐Ming Yan
出处
期刊:ACS Nano [American Chemical Society]
卷期号:17 (14): 13974-13984 被引量:72
标识
DOI:10.1021/acsnano.3c03952
摘要

Efficient conversion of carbon dioxide (CO2) into value-added materials and feedstocks, powered by renewable electricity, presents a promising strategy to reduce greenhouse gas emissions and close the anthropogenic carbon loop. Recently, there has been intense interest in Cu2O-based catalysts for the CO2 reduction reaction (CO2RR), owing to their capabilities in enhancing C–C coupling. However, the electrochemical instability of Cu+ in Cu2O leads to its inevitable reduction to Cu0, resulting in poor selectivity for C2+ products. Herein, we propose an unconventional and feasible strategy for stabilizing Cu+ through the construction of a Ce4+ 4f–O 2p–Cu+ 3d network structure in Ce-Cu2O. Experimental results and theoretical calculations confirm that the unconventional orbital hybridization near Ef based on the high-order Ce4+ 4f and 2p can more effectively inhibit the leaching of lattice oxygen, thereby stabilizing Cu+ in Ce-Cu2O, compared with traditional d–p hybridization. Compared to pure Cu2O, the Ce-Cu2O catalyst increased the ratio of C2H4/CO by 1.69-fold during the CO2RR at −1.3 V. Furthermore, in situ and ex situ spectroscopic techniques were utilized to track the oxidation valency of copper under CO2RR conditions with time resolution, identifying the well-maintained Cu+ species in the Ce-Cu2O catalyst. This work not only presents an avenue to CO2RR catalyst design involving the high-order 4f and 2p orbital hybridization but also provides deep insights into the metal-oxidation-state-dependent selectivity of catalysts.
最长约 10秒,即可获得该文献文件

科研通智能强力驱动
Strongly Powered by AbleSci AI
更新
PDF的下载单位、IP信息已删除 (2025-6-4)

科研通是完全免费的文献互助平台,具备全网最快的应助速度,最高的求助完成率。 对每一个文献求助,科研通都将尽心尽力,给求助人一个满意的交代。
实时播报
共享精神应助Salt采纳,获得10
1秒前
糖糖发布了新的文献求助10
1秒前
打打应助欧维采纳,获得10
2秒前
LSJ完成签到,获得积分10
3秒前
3秒前
开开心心发布了新的文献求助10
3秒前
谦让雨柏完成签到,获得积分10
4秒前
minion完成签到,获得积分10
5秒前
5秒前
5秒前
5秒前
dzbb发布了新的文献求助10
7秒前
zhaoyuyuan发布了新的文献求助10
7秒前
彭于晏应助梦想在飞采纳,获得10
7秒前
8秒前
宇宙大静默完成签到 ,获得积分10
9秒前
淡定的黑米完成签到,获得积分10
9秒前
Ing发布了新的文献求助10
9秒前
Orange应助芷莯采纳,获得10
10秒前
苗大楚发布了新的文献求助100
10秒前
10秒前
axn发布了新的文献求助10
11秒前
11秒前
11秒前
石夜一觞发布了新的文献求助10
12秒前
tinneywu发布了新的文献求助10
12秒前
NexusExplorer应助zhaoyuyuan采纳,获得10
13秒前
大个应助科研通管家采纳,获得10
14秒前
赘婿应助科研通管家采纳,获得10
14秒前
所所应助科研通管家采纳,获得10
14秒前
14秒前
科研通AI2S应助科研通管家采纳,获得30
14秒前
wy.he应助科研通管家采纳,获得50
14秒前
14秒前
14秒前
14秒前
15秒前
Orange应助科研通管家采纳,获得10
15秒前
15秒前
15秒前
高分求助中
Picture Books with Same-sex Parented Families: Unintentional Censorship 700
ACSM’s Guidelines for Exercise Testing and Prescription, 12th edition 500
Nucleophilic substitution in azasydnone-modified dinitroanisoles 500
不知道标题是什么 500
Indomethacinのヒトにおける経皮吸収 400
Phylogenetic study of the order Polydesmida (Myriapoda: Diplopoda) 370
Effective Learning and Mental Wellbeing 300
热门求助领域 (近24小时)
化学 材料科学 医学 生物 工程类 有机化学 生物化学 物理 内科学 纳米技术 计算机科学 化学工程 复合材料 遗传学 基因 物理化学 催化作用 冶金 细胞生物学 免疫学
热门帖子
关注 科研通微信公众号,转发送积分 3974844
求助须知:如何正确求助?哪些是违规求助? 3519270
关于积分的说明 11197844
捐赠科研通 3255496
什么是DOI,文献DOI怎么找? 1797791
邀请新用户注册赠送积分活动 877187
科研通“疑难数据库(出版商)”最低求助积分说明 806202