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One-Step Approach for Constructing High-Density Single-Atom Catalysts toward Overall Water Splitting at Industrial Current Densities |
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| Authors: | Dr Dong Cao Dr Zhirong Zhang Yahui Cui Runhao Zhang Prof Lipeng Zhang Prof Jie Zeng Prof Daojian Cheng |
| Institution: | 1. State Key Laboratory of Organic-Inorganic Composites and Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029 P. R. China
These authors contributed equally to this work.;2. School of Chemistry & Chemical Engineering, Anhui University of Technology, Ma'anshan, Anhui 243002 P. R. China Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026 P. R. China These authors contributed equally to this work.;3. State Key Laboratory of Organic-Inorganic Composites and Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029 P. R. China;4. Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026 P. R. China;5. School of Chemistry & Chemical Engineering, Anhui University of Technology, Ma'anshan, Anhui 243002 P. R. China |
| Abstract: | The construction of highly active, durable, and cost-effective catalysts is urgently needed for green hydrogen production. Herein, catalysts consisting of high-density Pt (24 atoms nm−2) and Ir (32 atoms nm−2) single atoms anchored on Co(OH)2 were constructed by a facile one-step approach. Remarkably, Pt1/Co(OH)2 and Ir1/Co(OH)2 only required 4 and 178 mV at 10 mA cm−2 for hydrogen evolution reaction and oxygen evolution reaction, respectively. Moreover, the assembled Pt1/Co(OH)2//Ir1/Co(OH)2 system showed mass activity of 4.9 A mgnoble metal−1 at 2.0 V in an alkaline water electrolyzer, which is 316.1 times higher than that of Pt/C//IrO2. Mechanistic studies revealed that reconstructed Ir−O6 single atoms and remodeled Pt triple-atom sites enhanced the occupancy of Ir−O bonding orbitals and improved the occupation of Pt−H antibonding orbital, respectively, contributing to the formation of the O−O bond and the desorption of hydrogen. This one-step approach was also generalized to fabricate other 20 single-atom catalysts. |
| Keywords: | Hydrogen Evolution Reaction Oxygen Evolution Reaction Reaction Mechanisms Single-Atom Catalysts |