摘要
It is of great interest to develop the novel transition metal-based electrocatalysts with high selectivity and activity for two electron oxygen reduction reaction(2e^(-) ORR).Herein,the nickel ditelluride(NiTe_(2)) with layered structure was explored as the 2e^(-) ORR electrocatalyst,which not only showed the highest 2e^(-) selectivity more than 97%,but also delivered a slight activity decay after 5000 cycles in alkaline media.Moreover,when NiTe_(2) was assembled as the electrocatalyst in H-type electrolyzer,the on-site yield of H_(2)O_(2) could reach up to 672 mmol h^(-1)g^(-1) under 0.45 V vs.RHE.Further in situ Raman spectra,theoretical calculation and post microstructural analysis synergistically unveiled that such a good 2e^(-) ORR performance could be credited to the intrinsic layered crystal structure,the high compositional stability,as well as the electron modulation on the active site Ni atoms by neighboring Te atoms,leading to the exposure of active sites as well as the optimized adsorption free energy of Ni to –OOH.More inspiringly,such telluride electrocatalyst has also been demonstrated to exhibit high activity and selectivity towards 2e^(-) ORR in neutral media.
基金
supported by the National MCF Energy R&D Program of China (2018YFE0306105)
the National Key R&D Program of China (2020YFA0406104, 2020YFA0406101)
the Innovative Research Group Project of the National Natural Science Foundation of China (51821002)
the National Natural Science Foundation of China (52201269, 52302296, 51972216)
the Natural Science Foundation of Jiangsu Province (BK20220028, BK20210735)
the Natural Science Foundation of the Higher Education Institutions of Jiangsu Province (21KJB430043)
the Collaborative Innovation Center of Suzhou Nano Science & Technology, the 111 Project
the Suzhou Key Laboratory of Functional Nano & Soft Materials, the Jiangsu Key Laboratory for Advanced Negative Carbon Technologies
the Science and Technology Development Fund, Macao SAR (0009/2022/ITP)
the funding from Gusu leading talent plan for scientific and technological innovation and entrepreneurship (ZXL2022487)
China Scholarship Council (CSC) for the Ph.D. fellowship。
