广东石油化工大学Xiangming Li研究小组通过氮化石墨碳负载的金属-有机笼型修饰金纳米颗粒，促进了纯水压电催化生产H₂O₂。2023年11月20日，《德国应用化学》杂志发表了这一成果。

在该研究中，金属有机笼包裹的金纳米颗粒通过氢键固定在石墨氮化碳(MOC-AuNP/g-C₃N₄)上，作为高效生成H₂O₂的多功能位点。实验和理论计算证明，MOC-AuNP/g-C₃N₄同时优化了压电催化制H₂O₂的三个关键环节：1) MOC组分通过主客体相互作用增强了对底物(O₂)和产物(H₂O₂)的吸附，阻碍了H₂O₂在MOC-AuNP/g-C₃N₄上的快速分解；2)AuNP组分提供了强大的界面电场，显著促进了g-C₃N₄的电子迁移进行O₂还原反应(ORR)；3)空穴用于H₂O氧化反应(WOR)产生O₂和H+，进一步促进ORR。MOC-AuNP/g-C₃N₄可以作为一种高效的压电催化剂，在空气和纯水中以高达120.21 μmol g^-1 h^-1的速率生成H₂O₂，而无需使用牺牲剂。该研究提出了一种新的策略，通过氢键在半导体催化剂上构建多个活性位点，增强底物吸附，快速分离电子空穴对，防止H₂O₂的快速分解，从而有效地催化合成H₂O₂。

据了解，压电催化生产过氧化氢(H₂O₂)是一种绿色合成方法，但压电催化剂中载流子的快速络合和吸附底物的困难限制了其性能。

附：英文原文

Title: Promoting Piezocatalytic H2O2 Production in Pure Water by Loading Metal-Organic Cage-Modified Gold Nanoparticles on Graphitic Carbon Nitride

Author: Meng Fu, Jinghong Luo, Bo Shi, Shuchen Tu, Zihao Wang, Changlin Yu, Zequn Ma, Xingyuan Chen, Xiangming Li

Issue&Volume: 2023-11-20

Abstract: Piezocatalytic hydrogen peroxide (H2O2) production is a green synthesis method, but the rapid complexation of charge carriers in piezocatalysts and the difficulty of adsorbing substrates limit its performance. Here, metal-organic cage-coated gold nanoparticles are anchored on graphitic carbon nitride (MOC-AuNP/g-C3N4) via hydrogen bond to serve as the multifunctional sites for efficient H2O2 production. Experiments and theoretical calculations prove that MOC-AuNP/g-C3N4 simultaneously optimize three key parts of piezocatalytic H2O2 production: i) the MOC component enhances substrate (O2) and product (H2O2) adsorption via host-guest interaction and hinders the rapid decomposition of H2O2 on MOC-AuNP/g-C3N4, ii) the AuNP component affords a strong interfacial electric field that significantly promotes the migration of electrons from g-C3N4 for O2 reduction reaction (ORR), iii) holes are used for H2O oxidation reaction (WOR) to produce O2 and H+ to further promote ORR. Thus, MOC-AuNP/g-C3N4 can be used as an efficient piezocatalyst to generate H2O2 at rates up to 120.21 μmol g-1 h-1 in air and pure water without using sacrificial agents. This work proposes a new strategy for efficient piezocatalytic H2O2 synthesis by constructing multiple active sites in semiconductor catalysts via hydrogen bonding, by enhancing substrate adsorption, rapid separation of electron-hole pairs and preventing rapid decomposition of H2O2.

DOI: 10.1002/anie.202316346

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202316346