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Cooperative Ni(Co)-Ru-P Sites Activate Dehydrogenation for Hydrazine Oxidation Assisting Self-powered H2 Production |
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| Authors: | Yanmin Hu Tingting Chao Yapeng Li Peigen Liu Tonghui Zhao Ge Yu Cai Chen Xiao Liang Huile Jin Shuwen Niu Wei Chen Dingsheng Wang Yadong Li |
| Institution: | 1. Key Laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035 China
Center of Advanced Nanocatalysis (CAN), Department of Applied Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, 230026 China These authors contributed equally to this work.;2. Key Laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035 China These authors contributed equally to this work.;3. Center of Advanced Nanocatalysis (CAN), Department of Applied Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, 230026 China These authors contributed equally to this work.;4. Key Laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035 China;5. Center of Advanced Nanocatalysis (CAN), Department of Applied Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, 230026 China;6. Department of Chemistry, Tsinghua University, Beijing, China |
| Abstract: | Water electrolysis for H2 production is restricted by the sluggish oxygen evolution reaction (OER). Using the thermodynamically more favorable hydrazine oxidation reaction (HzOR) to replace OER has attracted ever-growing attention. Herein, we report a twisted NiCoP nanowire array immobilized with Ru single atoms (Ru1−NiCoP) as superior bifunctional electrocatalyst toward both HzOR and hydrogen evolution reaction (HER), realizing an ultralow working potential of −60 mV and overpotential of 32 mV for a current density of 10 mA cm−2, respectively. Inspiringly, two-electrode electrolyzer based on overall hydrazine splitting (OHzS) demonstrates outstanding activity with a record-high current density of 522 mA cm−2 at cell voltage of 0.3 V. DFT calculations elucidate the cooperative Ni(Co)−Ru−P sites in Ru1−NiCoP optimize H* adsorption, and enhance adsorption of *N2H2 to significantly lower the energy barrier for hydrazine dehydrogenation. Moreover, a self-powered H2 production system utilizing OHzS device driven by direct hydrazine fuel cell (DHzFC) achieve a satisfactory rate of 24.0 mol h−1 m−2. |
| Keywords: | Dehydrogenation Hydrazine Oxidation Reaction Interfacial Sites Overall Hydrazine Splitting Single-Atom Catalyst |