Tuning the Properties of N-Doped Biochar for Selective CO2 Electroreduction to CO

被引:32
作者
Fu, Shilong [1 ]
Li, Ming [1 ,2 ]
de Jong, Wiebren [1 ]
Kortlever, Ruud [1 ]
机构
[1] Delft Univ Technol, Fac Mech Maritime & Mat Engn, Large Scale Energy Storage Proc & Energy Dept, NL-2628 CB Delft, Netherlands
[2] Delft Univ Technol, Fac Appl Sci, Chem Engn Dept, Prod & Proc Engn, NL-2628 HZ Delft, Netherlands
关键词
CO2 electrochemical reduction; N-doped carbon; carbon-based electrocatalysts; structure-performancecorrelation; electrocatalysis; POROUS CARBON; MESOPOROUS CARBON; HIGHLY EFFICIENT; NITROGEN; REDUCTION; DIOXIDE; BIOMASS; ACTIVATION; ELECTROCATALYST; OPPORTUNITIES;
D O I
10.1021/acscatal.3c01773
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
Nitrogen-doped (N-doped)carbon catalysts have been widely studiedfor electrochemical CO2 reduction to CO. However, the correlationbetween the physicochemical properties of N-doped carbon catalystsand their electrocatalytic performance for the CO2RR isstill unclear. Herein, a series of N-doped biochar catalysts withdifferent physicochemical properties were synthesized by tuning thecarbonization temperature and N-doping level and used for the CO2RR to analyze the structure-performance relationship.The prepared catalysts exhibited massive differences in maximum faradaicefficiency to CO from 26.8 to 94.9% at around -0.8 to -0.9V vs RHE. In addition, we find that simply increasing the specificsurface area and N-doping level of the catalysts does not effectivelyimprove the catalytic performance for the CO2RR. A multivariatecorrelation analysis reveals a negative correlation between the N-dopingcontent and the electrochemical performance. The porous structuralproperties exhibit a positive correlation to the FECO butalmost no correlation to j (CO). Interestingly,improving the degree of graphitization, surface hydrophobicity, theabundance of defects, and optimizing the porosity of the N-doped biocharcatalyst can efficiently enhance the catalytic performance for theCO(2)RR. We conclude that comprehensively analyzing the synergisticeffect of various properties of N-doped biochar is critical to revealstructure-activity relationships.
引用
收藏
页码:10309 / 10323
页数:15
相关论文
共 55 条
[1]   Carbon-based electrocatalysts for CO2 electroreduction produced via MOF, biomass, and other precursors carbonization: A review [J].
Abdelkader-Fernandez, Victor K. ;
Fernandes, Diana M. ;
Freire, Cristina .
JOURNAL OF CO2 UTILIZATION, 2020, 42
[2]   Electrochemical CO2 conversion to fuels on metal-free N-doped carbon-based materials: functionalities, mechanistic, and technoeconomic aspects [J].
Adegoke, Kayode Adesina ;
Maxakato, Nobanathi Wendy .
MATERIALS TODAY CHEMISTRY, 2022, 24
[3]   Deconvoluting the XPS spectra for nitrogen-doped chars: An analysis from first principles [J].
Ayiania, Michael ;
Smith, Matthew ;
Hensley, Alyssa J. R. ;
Scudiero, Louis ;
McEwen, Jean-Sabin ;
Garcia-Perez, Manuel .
CARBON, 2020, 162 :528-544
[4]   Progress toward Commercial Application of Electrochemical Carbon Dioxide Reduction [J].
Chen, Chi ;
Kotyk, Juliet F. Khosrowabadi ;
Sheehan, Stafford W. .
CHEM, 2018, 4 (11) :2571-2586
[5]  
Chmiola J, 2006, SCIENCE, V313, P1760, DOI [10.1126/science.1132195, 10.1126/science/1132195]
[6]   Opportunities and challenges for a sustainable energy future [J].
Chu, Steven ;
Majumdar, Arun .
NATURE, 2012, 488 (7411) :294-303
[7]   Selective Etching of Nitrogen-Doped Carbon by Steam for Enhanced Electrochemical CO2 Reduction [J].
Cui, Xiaoqi ;
Pan, Zhiyong ;
Zhang, Lijuan ;
Peng, Huisheng ;
Zheng, Gengfeng .
ADVANCED ENERGY MATERIALS, 2017, 7 (22)
[8]   Electroreduction of CO2 to CO on a Mesoporous Carbon Catalyst with Progressively Removed Nitrogen Moieties [J].
Daiyan, Rahman ;
Tan, Xin ;
Chen, Rui ;
Saputera, Wibawa Hendra ;
Tahini, Hassan A. ;
Lovell, Emma ;
Ng, Yun Hau ;
Smith, Sean C. ;
Dai, Liming ;
Lu, Xunyu ;
Amal, Rose .
ACS ENERGY LETTERS, 2018, 3 (09) :2292-2298
[9]   Unraveling the rate-limiting step of two-electron transfer electrochemical reduction of carbon dioxide [J].
Deng, Wanyu ;
Zhang, Peng ;
Seger, Brian ;
Gong, Jinlong .
NATURE COMMUNICATIONS, 2022, 13 (01)
[10]   Hierarchically Porous Carbon Materials for CO2 Capture: The Role of Pore Structure. [J].
Estevez, Luis ;
Barpaga, Dushyant ;
Zheng, Jian ;
Sabale, Sandip ;
Patel, Rajankumar L. ;
Zhang, Ji-Guang ;
McGrail, B. Peter ;
Motkuri, Radha Kishan .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2018, 57 (04) :1262-1268