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羟基化硼晶体域调制异质结构碳催化剂高效过氧化氢生成
作者:小柯机器人 发布时间:2025/6/14 17:20:24


近日,南京林业大学范孟孟团队研究了羟基化硼晶体域调制异质结构碳催化剂高效过氧化氢生成。这一研究成果发表在2025年6月11日出版的《美国化学会志》上。

无金属异质结构碳催化剂是通过双电子氧还原反应(2e-ORR)合成电化学过氧化氢(H2O2)的金属基催化剂的有前景的替代品。然而,人们正在寻求一种合适的纳米晶体类型来解决工业级电流密度的问题。在此,纳米硼晶畴(Bn)克服了传统碳基电催化剂在可持续H2O2生产和工业应用中的稳定性限制。 

Bn-C催化剂提供了多个活性位点,而纳米Bn具有O2富集效应,增强了ORR电催化过程中的传质。Bn-C在碱性/中性电解质中表现出非常高的质量活性(11.6/10.7 mol gcat-1 h-1),在高电流密度(>300 mA cm-2)下连续电解100小时时,活性和法拉第效率的损失可以忽略不计(超过90%)。密度泛函理论和原位拉曼实验表明,连接纳米Bn的-OH基团对碳基质中的B原子具有诱导作用,减轻了与*OOH中间体结合强度过强的问题。

附:英文原文

Title: Hydroxylated Boron Crystal Domain-Modulated Heterostructure Carbon Catalysts for Efficient Hydrogen Peroxide Generation

Author: Yuhan Wu, Qixin Yuan, Yuying Zhao, Kang Sun, Hao Sun, Kui Wang, Shengchun Hu, Geoffrey I. N. Waterhouse, Jingjie Wu, Ziyun Wang, Jianchun Jiang, Mengmeng Fan

Issue&Volume: June 11, 2025

Abstract: Metal-free heterostructure carbon catalysts are promising alternatives to metal-based catalysts for electrochemical hydrogen peroxide (H2O2) synthesis via the two-electron oxygen reduction reaction (2e– ORR). However, one appropriate nanocrystal type is being sought to resolve a concern at industrial-level current densities. Herein, nano boron crystal domains (Bn) overcame the stability limitations of traditional carbon-based electrocatalysts for sustainable H2O2 production and industrial application. A Bn–C catalyst offered multiple active sites, while the nano Bn imparted an O2 enrichment effect enhancing mass transfer during ORR electrocatalysis. The Bn–C exhibited a very high mass activity (11.6/10.7 mol gcat–1 h–1) in alkaline/neutral electrolytes and showed negligible loss in activity and Faradaic efficiency (over 90%) during 100 h continuous electrolysis at high current density (>300 mA cm–2). Density functional theory and in situ Raman experiments demonstrated that the –OH groups connecting nano Bn provided an inductive effect on B atoms in the carbon matrix, alleviating a binding strength that is too strong with *OOH intermediate.

DOI: 10.1021/jacs.5c03955

Source: https://pubs.acs.org/doi/abs/10.1021/jacs.5c03955

期刊信息

JACS:《美国化学会志》,创刊于1879年。隶属于美国化学会,最新IF:16.383
官方网址:https://pubs.acs.org/journal/jacsat
投稿链接:https://acsparagonplus.acs.org/psweb/loginForm?code=1000