Nickel single-atom catalysts intrinsically promoted by fast pyrolysis for selective electroreduction of CO2 into CO

被引:117
作者
Guo, Yibo [1 ]
Yao, Sai [1 ]
Xue, Yuanyuan [1 ]
Hu, Xu [1 ]
Cui, Huijuan [2 ]
Zhou, Zhen [1 ,3 ]
机构
[1] Nankai Univ, Renewable Energy Convers & Storage Ctr ReCast, Key Lab Adv Energy Mat Chem, Minist Educ,Inst New Energy Mat Chem,Sch Mat Sci, Tianjin 300350, Peoples R China
[2] Chinese Acad Sci, Tianjin Inst Ind Biotechnol, Tianjin Airport Econ Area, 32 West 7th Ave, Tianjin 300308, Peoples R China
[3] Zhengzhou Univ, Engn Res Ctr Adv Funct Mat Mfg, Sch Chem Engn, Minist Educ, Zhengzhou 450001, Peoples R China
来源
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2022年 / 304卷
基金
中国国家自然科学基金;
关键词
Nickel single-atom catalysts; Fast pyrolysis; Electrocatalysis; Carbon dioxide reduction; Carbon neutralization; ELECTROCATALYTIC ACTIVITY; REDUCTION;
D O I
10.1016/j.apcatb.2021.120997
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The electrochemical reduction reaction of carbon dioxide (CO2RR) is an effective way towards carbon neutralization. Single-atom catalysts (SACs) are expected to be efficient for CO2RR due to maximum atom utilization and excellent catalytic performance. Here, nitrogen-doped carbon supported Ni SACs (Ni-SAC@NCs) were prepared through effective fast pyrolysis. CO2 can convert into CO efficiently with Ni-SAC@NCs as electrocatalysts for CO2RR. The faradaic efficiency kept well above 80% in the applied potential window of -0.6 to -0.9 V (vs. reversible hydrogen electrode (RHE)), with a highest FECO of 95% at -0.6 V (vs. RHE). Ni-SAC@NCs can achieve the best CO selectivity under a small overpotential, surpassing most other state-of-the-art catalysts. Computations also indicate that the unique defect-Ni-N-3 structure is the active site. This work not only provides a simple and promising new route for the preparation of SACs, but also proves the key role of the coordination environment in electrocatalysis.
引用
收藏
页数:8
相关论文
共 43 条
[1]   Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels [J].
Birdja, Yuvraj Y. ;
Perez-Gallent, Elena ;
Figueiredo, Marta C. ;
Gottle, Adrien J. ;
Calle-Vallejo, Federico ;
Koper, Marc T. M. .
NATURE ENERGY, 2019, 4 (09) :732-745
[2]   Theoretical Considerations on the Electroreduction of CO to C2 Species on Cu(100) Electrodes [J].
Calle-Vallejo, Federico ;
Koper, Marc T. M. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2013, 52 (28) :7282-7285
[3]   Unsaturated edge-anchored Ni single atoms on porous microwave exfoliated graphene oxide for electrochemical CO2 [J].
Cheng, Yi ;
Zhao, Shiyong ;
Li, Haobo ;
He, Shuai ;
Veder, Jean-Pierre ;
Johannessen, Bernt ;
Xiao, Jianping ;
Lu, Shanfu ;
Pan, Jian ;
Chisholm, Mattew F. ;
Yang, Shi-Ze ;
Liu, Chang ;
Chen, Jingguang G. ;
Jiang, San Ping .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2019, 243 :294-303
[4]   2 D Materials for Electrochemical Energy Storage: Design, Preparation, and Application [J].
Cui, Huijuan ;
Guo, Yibo ;
Ma, Wei ;
Zhou, Zhen .
CHEMSUSCHEM, 2020, 13 (06) :1155-1171
[5]   Heteroatom-doped carbon materials and their composites as electrocatalysts for CO2 reduction [J].
Cui, Huijuan ;
Guo, Yibo ;
Guo, Limin ;
Wang, Liang ;
Zhou, Zhen ;
Peng, Zhangquan .
JOURNAL OF MATERIALS CHEMISTRY A, 2018, 6 (39) :18782-18793
[6]   Transforming active sites in nickel-nitrogen-carbon catalysts for efficient electrochemical CO2 reduction to CO [J].
Daiyan, Rahman ;
Zhu, Xiaofeng ;
Tong, Zizheng ;
Gong, Lele ;
Razmjou, Amir ;
Liu, Ru-Shi ;
Xia, Zhenhai ;
Lu, Xunyu ;
Dai, Liming ;
Amal, Rose .
NANO ENERGY, 2020, 78
[7]   Activation of Ni Particles into Single Ni-N Atoms for Efficient Electrochemical Reduction of CO2 [J].
Fan, Qun ;
Hou, Pengfei ;
Choi, Changhyeok ;
Wu, Tai-Sing ;
Hong, Song ;
Li, Fang ;
Soo, Yun-Liang ;
Kang, Peng ;
Jung, Yousung ;
Sun, Zhenyu .
ADVANCED ENERGY MATERIALS, 2020, 10 (05)
[8]   A Mn-N3 single-atom catalyst embedded in graphitic carbon nitride for efficient CO2 electroreduction [J].
Feng, Jiaqi ;
Gao, Hongshuai ;
Zheng, Lirong ;
Chen, Zhipeng ;
Zeng, Shaojuan ;
Jiang, Chongyang ;
Dong, Haifeng ;
Liu, Licheng ;
Zhang, Suojiang ;
Zhang, Xiangping .
NATURE COMMUNICATIONS, 2020, 11 (01)
[9]   Accuracy of exchange-correlation functionals and effect of solvation on the surface energy of copper [J].
Fishman, Matthew ;
Zhuang, Houlong L. ;
Mathew, Kiran ;
Dirschka, William ;
Hennig, Richard G. .
PHYSICAL REVIEW B, 2013, 87 (24)
[10]   Regulating the coordination environment of Co single atoms for achieving efficient electrocatalytic activity in CO2 reduction [J].
Geng, Zhigang ;
Cao, Yuanjie ;
Chen, Wenxing ;
Kong, Xiangdong ;
Liu, Yan ;
Yao, Tao ;
Lin, Yue .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2019, 240 :234-240