Ligand-Hybridization Engineering Enabling Stable Cuδ+ for Durable CO2 Electroreduction to C2+ Products

被引:0
作者
Lu, Youluan [1 ]
Zhang, Jingfang [1 ,2 ]
Wu, Danyang [1 ]
Liu, Yue [1 ]
Qiu, Mingyue [1 ]
Sun, Deyun [1 ]
Wu, Haonan [1 ]
Yi, Qun [1 ]
机构
[1] Wuhan Inst Technol, Sch Chem Engn & Pharm, Minist Educ, Key Lab Green Chem Engn Proc, Wuhan 430072, Peoples R China
[2] Nankai Univ, Key Lab Adv Energy Mat Chem, Minist Educ, Tianjin 300071, Peoples R China
基金
中国国家自然科学基金;
关键词
C2+ products; CO2; electroreduction; Cu; ligand hybridization; CARBON-DIOXIDE ELECTROREDUCTION; COPPER; REDUCTION;
D O I
10.1002/adfm.202512342
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Electrocatalytic carbon dioxide reduction reaction (CO2RR) offers a sustainable route to convert CO2 into value-added multi-carbon (C2+) chemicals using renewable electricity. Copper (Cu) is considered as the promising catalyst for generating C2+ products, but suffers from low Faradaic efficiency (FE) and poor stability. Herein, a ligand-hybridization strategy on Cu-2(OH)(3)NO3 (CuON) to precisely regulate the coordination environment of Cu sites by partially substituting hydroxyl or nitrate with acetate ligands is demonstrated. The ligand hybridization facilitates the electron delocalization across Cu sites and the coordinated acetate ligands, and induces the formation and stabilization of active Cu delta+ species, thereby boosting efficient and stable C-C coupling for selective C2+ production. Impressively, acetate-hybridized CuON catalyst (AH-CuON) exhibits superior FE up to 74.7% at a high current density of 400 mA cm(-2) toward C2+ products, while maintaining stability for 20 h toward CO2RR. Significantly, this study offers a new strategy for designing highly efficient and stable Cu-based CO2RR catalysts toward C2+ products.
引用
收藏
页数:8
相关论文
共 52 条
[1]  
C.S. of Electrochemistry, 2024, J. Electrochem., V30, DOI [10.61558/2993-074x.3444, DOI 10.61558/2993-074X.3444]
[2]   Two Birds with One Stone: Guanidyl Carbon Dots with Enhanced Antioxidative and Lipolytic Functions in Metabolic Associated Fatty Liver [J].
Cai, Hao ;
Li, Yan ;
Wu, Xiaoyan ;
Yang, Yuxiang ;
Tedesco, Antonio Claudio ;
Li, Zijian ;
Bi, Hong .
ADVANCED FUNCTIONAL MATERIALS, 2024, 34 (45)
[3]   Shielding effect in the synthesis of Gd-doped copper oxide catalysts with enhanced CO2 electroreduction to ethylene [J].
Cao, Zenan ;
Chen, Zhichao ;
Sun, Hanlei ;
Yao, Shuo ;
Liu, Ziyong ;
Li, Fuli ;
Yang, Xiaobo ;
Zhou, Wei ;
Fan, Jingxin ;
Wang, Hongzhi ;
Liu, Licheng .
JOURNAL OF MATERIALS CHEMISTRY A, 2024, 12 (42) :29165-29173
[4]   Supported Au single atoms and nanoparticles on MoS2 for highly selective CO2-to-CH3COOH photoreduction [J].
Chen, Cai ;
Ye, Chunyin ;
Zhao, Xinglei ;
Zhang, Yizhen ;
Li, Ruilong ;
Zhang, Qun ;
Zhang, Hui ;
Wu, Yuen .
NATURE COMMUNICATIONS, 2024, 15 (01)
[5]   Ultrathin Hydrogel Films toward Breathable Skin-Integrated Electronics [J].
Cheng, Simin ;
Lou, Zirui ;
Zhang, Lan ;
Guo, Haotian ;
Wang, Zitian ;
Guo, Chuanfei ;
Fukuda, Kenjiro ;
Ma, Shaohua ;
Wang, Guoqing ;
Someya, Takao ;
Cheng, Hui-Ming ;
Xu, Xiaomin .
ADVANCED MATERIALS, 2023, 35 (01)
[6]   Controlling the Oxidation State of the Cu Electrode and Reaction Intermediates for Electrochemical CO2 Reduction to Ethylene [J].
Chou, Tsu-Chin ;
Chang, Chiao-Chun ;
Yu, Hung-Ling ;
Yu, Wen-Yueh ;
Dong, Chung-Li ;
Velasco-Velez, Juan Jesus ;
Chuang, Cheng-Hao ;
Chen, Li-Chyong ;
Lee, Jyh-Fu ;
Chen, Jin-Ming ;
Wu, Heng-Liang .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2020, 142 (06) :2857-2867
[7]   In Situ Infrared Spectroscopic Evidence of Enhanced Electrochemical CO2 Reduction and C-C Coupling on Oxide-Derived Copper [J].
Delmo, Ernest Pahuyo ;
Wang, Yian ;
Song, Yihua ;
Zhu, Shangqian ;
Zhang, Haichuan ;
Xu, Hongming ;
Li, Tiehuai ;
Jang, Juhee ;
Kwon, Yongjun ;
Wang, Yinuo ;
Shao, Minhua .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2024, 146 (03) :1935-1945
[8]  
Deng J., 2024, Small, V20
[9]   In Situ Raman Spectroscopy of Copper and Copper Oxide Surfaces during Electrochemical Oxygen Evolution Reaction: Identification of CuIII Oxides as Catalytically Active Species [J].
Deng, Yilin ;
Handoko, Albertus D. ;
Du, Yonghua ;
Xi, Shibo ;
Yeo, Boon Siang .
ACS CATALYSIS, 2016, 6 (04) :2473-2481
[10]  
Duan G. Y., 2022, Angew. Chem., V134