文献类型：期刊文献

英文题名：Pyrolysis-Free Mechanochemical Conversion of Small Organic Molecules into Metal-Free Heteroatom-Doped Mesoporous Carbons for Efficient Electrosynthesis of Hydrogen Peroxide

作者：Yang, Na[1,2];Zhu, Xiang[1,2];Wang, Guofeng[1,2];Zhou, Lulu[3];Zhu, Xiaoxiao[3];Pan, Jiaqi[3];Yu, Wei[4];Xia, Chungu[1,2];Tian, Chengcheng[3]

机构：[1]Chinese Acad Sci, Suzhou Res Inst LICP, Lanzhou Inst Chem Phys LICP, State Key Lab Oxo Synth & Select Oxidat OSSO, Lanzhou 730000, Peoples R China;[2]Univ Chinese Acad Sci, Beijing 100049, Peoples R China;[3]East China Univ Sci & Technol, Sch Resources & Environm Engn, Shanghai 200237, Peoples R China;[4]Jiangnan Univ, Jiangsu Key Lab Adv Food Mfg Equipment & Technol, Wuxi 214122, Peoples R China

年份：2023

卷号：5

期号：2

起止页码：379

外文期刊名：ACS MATERIALS LETTERS

收录：;EI(收录号：20230313387800);WOS:【SCI-EXPANDED(收录号:WOS:000911970900001)】；

基金：X.Z. thanks the National Program for Young Talents of China and National Natural Science Foundation of China (E00966GMS1 and E00966GZQ2) for financial support. C.T. was supported by Shanghai International Science and Technology Cooperation Project (20230710700), the Shanghai Science and technology Innovation Plan (22dz1208600), and the National Natural Science Foundation of China (52170109).

语种：英文

外文关键词：Ball milling - Carbon - Electrocatalysts - Electrolytic reduction - Ketones - Mesoporous materials - Molecules - Oxidation - Potassium hydroxide - Pyrolysis

摘要：The synthesis of heteroatom-doped porous carbons for efficient electrochemical production of hydrogen peroxide (H2O2) through two-electron (2e(-)) oxygen reduction reaction (ORR) has attracted increasing research attention since it offers a promising renewable substitute for the traditional complex energy-intensive anthraquinone process. Herein, a novel pyrol-ysis-free mechanochemical approach was developed for straight-forward conversion of small organic molecules into metal-free heteroatom-doped mesoporous carbons (HMCs), where the uniqueness of this one-pot ball-milling technique not only exceeds the limit of volatilities of traditional carbonaceous precursors but also eliminates the need for any additional mesoporous templates. The abundance of molecular precursors (up to 23 different molecules) provides a facile means to introduce a wide variety of heteroatoms (B, N, O, P, S, F, Cl, etc.) into the resultant carbon materials, accompanied by in situ formation of rich mesopores. As a result, the resulting N/O co-doped mesoporous carbon with the highest Brunauer-Emmett-Teller (BET) surface area of 1238 m(2) g(-1) exhibits exceptional H2O2 selectivity of 95.2% in 0.1 M KOH solution at 0.70 V (vs. reversible hydrogen electrode, RHE) and a large H2O2 production rate of ca. 265 mmol g(cat.)(-1) h(-1), ranking at the top among all metal-free carbonaceous electrocatalysts. We anticipate our findings will facilitate new possibilities for the development of mesoporous carbons for electrocatalytic applications.