Elevated temperature-driven coordinative reconstruction of an unsaturated single-Ni-atom structure with low valency on a polymer-derived matrix for the electrolytic oxygen evolution reaction

作     者：Patil, Rahul Rajput, Anubha Matsagar, Babasaheb M. Chen, Norman C. R. Ujihara, Masaki Salunkhe, Rahul R. Yadav, Praveen Wu, Kevin C.-W. Chakraborty, Biswarup Dutta, Saikat 

作者机构：Electrochemical Energy & Sensor Research Laboratory Amity Institute of Click Chemistry Research & Studies Amity University Noida India Department of Chemistry Indian Institute of Technology New Delhi India Department of Chemical Engineering National Taiwan University Taipei10617 Taiwan Molecular Science and Technology Program Taiwan International Graduate Program Academia Sinica Taiwan  National Taiwan University Taiwan Graduate Institute of Applied Science and Technology National Taiwan University of Science and Technology Taipei Taiwan Materials Research Laboratory Department of Physics Indian Institute of Technology Jammu India Synchrotron X-ray Facility Raja Ramanna Centre for Advanced Technology Rajendra Nagar Madhya Pradesh 452013 Indore India 

出 版 物：《Nanoscale》 (Nanoscale)

年 卷 期：2024年第16卷第15期

页      面：7467-7479页

核心收录：

学科分类：080701[工学-工程热物理] 0809[工学-电子科学与技术（可授工学、理学学位）] 07[理学] 0817[工学-化学工程与技术] 0807[工学-动力工程及工程热物理] 070203[理学-原子与分子物理] 0703[理学-化学] 0702[理学-物理学] 

基　　金：SD wishes to acknowledge research funding support by the Science & Engineering Research Board (SERB)  Department of Science & Technology  Government of India for support through core research grant number CRG/2023/000044 (2024–2027). SD also wishes to thank Department of Biotechnology  Ministry of Science & Technology  Government of India for a DBT Ramalingaswami Re-entry Fellowship grant number BT/RLF/Re-entry/41/2017 (2019–2024) and DBT-Energy Bioscience-Biofuels research grant number BT/PR38594/PBD/26/795/2020 (2023–2026). SD thanks the UGC-DAE Consortium for Scientific Research for a project under Collaborative Research Scheme (CRS) project grant number CRS/2022-23/01/680 (2023–2026) and Raja Rammana Centre for Advance Technology  Indore Beam Line 3 and 9 for soft and hard X-ray absorption spectroscopy. The authors would like to acknowledge NSRRC  Taiwan  Dr Chan  Ting-Shan  and Dr Pao  Chih-Wen for providing beamtimes and facilitating the SWLS-EXAFS experiments 

主　　题：Reaction kinetics 

摘      要：A high-temperature pyrolysis-controlled coordination reconstruction resulted in a single-Ni-atom structure with a Ni-Nx-C structural unit (x = N atom coordinated to Ni). Pyrolysis of Ni-phen@ZIF-8-RF at 700 °C resulted in NiNP-NC-700 with predominantly Ni nanoparticles. Upon elevating the pyrolysis temperature from 700 to 900 °C, a coordination reconstruction offers Ni-Nx atomic sites in NiSA-NC-900. A combined investigation with X-ray absorption spectroscopy, X-ray photoelectron spectroscopy, and soft X-ray L3-edge spectroscopy suggests the stabilization of low-valent Niδ+ (0 −2 was achieved. The cell potential recorded with Pt(−)/(+)NiSA-NC-900/NF was much lower than that obtained for other cells, i.e., Pt(−)/NF and NF(−)/(+)NF, which enhances the potentials of low-valent NiSAs for insightful understanding of the OER. At a constant applied potential of 1.61 V (vs. RHE) for 12 h, an small increase in current for initial 0.6 h followed by a constant current depicts the fair stability of catalyst for 12 h. Our results offer an insightful angle into the OER with a coordinatively reconstructed single-Ni-atom structure at lower valency ( © 2024 The Royal Society of Chemistry.