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Highly Efficient Metal-Free Coal-Based Carbon Aerogel Catalyst for Oxygen Reduction to Produce Hydrogen Peroxide
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2025-01-10 , DOI: 10.1021/acs.iecr.4c03929
Lingman Xia, Mingsheng Luo, Changke Shao, Zhi Yang, Huanqiao Song, Roshni Rahman, Ziyuan Li, Xiaoteng Cui, Wenshuai Yang
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2025-01-10 , DOI: 10.1021/acs.iecr.4c03929
Lingman Xia, Mingsheng Luo, Changke Shao, Zhi Yang, Huanqiao Song, Roshni Rahman, Ziyuan Li, Xiaoteng Cui, Wenshuai Yang
In this study, a highly efficient metal-free catalyst derived supported on coal-based carbon aerogel was successfully synthesized for the two-electron transfer oxygen reduction reaction (2e– ORR) to produce hydrogen peroxide (H2O2). The catalyst, with its high specific surface area and hierarchical porous structure, demonstrated exceptional selectivity for H2O2 under alkaline conditions. By optimization of the synthesis and drying conditions, particularly through the use of supercritical drying technology, the physicochemical properties and selectivity of the catalyst were significantly enhanced. Notably, the coal-based carbon gel obtained through supercritical drying with CO2 exhibited the superior specific surface area over 1311 m2·g–1. The H2O2 selectivity over 95% at a potential of 0.5 V vs SHE was obtained using the catalyst material synthesized from this study. It was also revealed that the high selectivity was attributed to the layered edge active sites, which are rich in carbonyl (C=O) and carboxyl (COOH) groups. In situ FTIR and Raman spectroscopic analyses confirmed the two-electron-transfer ORR reaction mechanism from this study.
中文翻译:
用于氧还原制得过氧化氢的高效无金属煤基碳气凝胶催化剂
在本研究中,成功合成了一种基于煤基碳气凝胶的高效无金属催化剂,用于双电子转移氧还原反应 (2e-ORR) 生成过氧化氢 (H2O2)。该催化剂具有高比表面积和多级多孔结构,在碱性条件下对 H2O2 表现出优异的选择性。通过优化合成和干燥条件,特别是通过使用超临界干燥技术,催化剂的物理化学性质和选择性得到了显著提高。值得注意的是,通过 CO2 超临界干燥获得的煤基碳凝胶表现出超过 1311 m2·g–1 的优异比表面积。使用本研究合成的催化剂材料,在 0.5 V vs SHE 的电位下,H2O2 选择性超过 95%。研究还发现,高选择性归因于层状边缘活性位点,这些位点富含羰基 (C=O) 和羧基 (COOH) 基团。原位 FTIR 和拉曼光谱分析证实了本研究的双电子转移 ORR 反应机制。
更新日期:2025-01-10
中文翻译:
用于氧还原制得过氧化氢的高效无金属煤基碳气凝胶催化剂
在本研究中,成功合成了一种基于煤基碳气凝胶的高效无金属催化剂,用于双电子转移氧还原反应 (2e-ORR) 生成过氧化氢 (H2O2)。该催化剂具有高比表面积和多级多孔结构,在碱性条件下对 H2O2 表现出优异的选择性。通过优化合成和干燥条件,特别是通过使用超临界干燥技术,催化剂的物理化学性质和选择性得到了显著提高。值得注意的是,通过 CO2 超临界干燥获得的煤基碳凝胶表现出超过 1311 m2·g–1 的优异比表面积。使用本研究合成的催化剂材料,在 0.5 V vs SHE 的电位下,H2O2 选择性超过 95%。研究还发现,高选择性归因于层状边缘活性位点,这些位点富含羰基 (C=O) 和羧基 (COOH) 基团。原位 FTIR 和拉曼光谱分析证实了本研究的双电子转移 ORR 反应机制。