The precise adjustment of the electronic structure of catalysts is an effective but difficult strategy for enhancing their catalytic performance. In this work, a defect engineering strategy was adopted to optimize the electronic structure of zeolitic imidazole zinc framework (ZIF)-derived in-situ nitrogen-doped carbon (N–C) via doping with nonmetal atoms (B and P/S). The doped nonmetal atoms altered the regular geometric construction of the catalyst and redistributed the electrons on the substrate, thus modifying the adsorption properties and catalytic ability of the catalyst. Benefitting from the modified electronic structure, enhanced structural defects, and synergistic effects among the different atoms, the N, B, and P/S co-doped carbon catalysts (BPN–C and BSN-C) exhibited enhanced catalytic activity. The best results were observed for BSN-C, which exhibited excellent catalytic activity for triiodide reduction reaction (IRR) in a photovoltaic device with an efficiency of 8.23%, superior to that of Pt (7.20%). BSN-C also produced a low overpotential of 129.7 mV at the current density of 10 mA cm⁻² in an alkaline hydrogen evolution reaction (HER). BPN-C and BSN-C displayed remarkable stability in the IRR and HER. This work presents a promising strategy for designing superior carbon-based metal-free catalysts via multivariate doping with non-metal heteroatoms for new energy applications.

精确调整催化剂的电子结构是提高其催化性能的一种有效但困难的策略。在这项工作中，采用缺陷工程策略，通过掺杂非金属原子（B和P/S）来优化沸石咪唑锌骨架（ZIF）衍生的原位氮掺杂碳（N-C）的电子结构。掺杂的非金属原子改变了催化剂的规则几何结构并重新分配了基底上的电子，从而改变了催化剂的吸附性能和催化能力。受益于改进的电子结构、增强的结构缺陷和不同原子之间的协同效应，N、B 和 P/S 共掺杂碳催化剂（BPN-C 和 BSN-C）表现出增强的催化活性。BSN-C 的结果最好，在光伏器件中表现出优异的三碘化物还原反应（IRR）催化活性，效率为8.23％，优于Pt（7.20％）。BSN-C 还在 10 mA cm 的电流密度下产生 129.7 mV 的低过电势^-2在碱性析氢反应 (HER) 中。BPN-C 和 BSN-C 在 IRR 和 HER 中表现出显着的稳定性。这项工作提出了一种很有前景的策略，可以通过非金属杂原子的多元掺杂来设计用于新能源应用的优质碳基无金属催化剂。