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Electrocatalytically Activating and Reducing N2 Molecule by Tuning Activity of Local Hydrogen Radical |
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| Authors: | Yuanyuan Yang Cejun Hu Dr Jieqiong Shan Chuanqi Cheng Prof Lili Han Prof Xinzhe Li Ruguang Wang Prof Wei Xie Prof Yao Zheng Prof Tao Ling |
| Institution: | 1. Key Laboratory for Advanced Ceramics and Machining Technology of Ministry of Education, Tianjin Key Laboratory of Composite and Functional Materials, School of Materials Science and Engineering, Tianjin University, Tianjin, 300072 China
These authors contributed equally to this work.;2. Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Tianjin Key Lab of Molecular Recognition & Biosensing, Renewable Energy Conversion and Storage Center College of Chemistry, Nankai University, Tianjin, 300071 China These authors contributed equally to this work.;3. School of Chemical Engineering, The University of Adelaide, Adelaide, SA 5005 Australia;4. Key Laboratory for Advanced Ceramics and Machining Technology of Ministry of Education, Tianjin Key Laboratory of Composite and Functional Materials, School of Materials Science and Engineering, Tianjin University, Tianjin, 300072 China;5. State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002 China;6. State Key Laboratory of Multiphase Flow in Power Engineering, School of Energy and Power Engineering, Xi'an Jiaotong University, Xi An Shi, Xi'an, 710049 China;7. Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Tianjin Key Lab of Molecular Recognition & Biosensing, Renewable Energy Conversion and Storage Center College of Chemistry, Nankai University, Tianjin, 300071 China |
| Abstract: | Decarbonizing N2 conversion is particularly challenging, but essential for sustainable development of industry and agriculture. Herein, we achieve electrocatalytic activation/reduction of N2 on X/Fe−N−C (X=Pd, Ir and Pt) dual-atom catalysts under ambient condition. We provide solid experimental evidence that local hydrogen radical (H*) generated on the X site of the X/Fe−N−C catalysts can participate in the activation/reduction of N2 adsorbed on the Fe site. More importantly, we reveal that the reactivity of X/Fe−N−C catalysts for N2 activation/reduction can be well adjusted by the activity of H* generated on the X site, i.e., the interaction between the X−H bond. Specifically, X/Fe−N−C catalyst with the weakest X−H bonding exhibits the highest H* activity, which is beneficial to the subsequent cleavage of X−H bond for N2 hydrogenation. With the most active H*, the Pd/Fe dual-atom site promotes the turnover frequency of N2 reduction by up to 10 times compared with the pristine Fe site. |
| Keywords: | Carbon Materials Electrocatalysis Metal-Free Catalysts Nitrogen Reduction Reaction |