通过反应界面微环境调控促进甲酸驱动的氧气还原合成过氧化氢
Boosting hydrogen peroxide production in formic acid-driven oxygen reduction via regulating the microenvironment of reaction interfaces
刘志萍 1盛夏 1陈茜 1卢净宇 1谭兆悦 1封心建2
作者信息
- 1. College of Chemistry,Chemical Engineering and Materials Science,Soochow University,Suzhou 215123,China
- 2. College of Chemistry,Chemical Engineering and Materials Science,Soochow University,Suzhou 215123,China;School of Chemistry and Materials Science,University of Science and Technology of China,Hefei 230026,China;Suzhou Institute for Advanced Research,University of Science and Technology of China,Suzhou 215123,China
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摘要
甲酸驱动的双电子氧还原是在温和条件下合成过氧化氢(H2O2)的一种很有前途的方法.然而,在传统的催化体系中,反应物O2在固体/液体两相反应界面处的浓度通常较低,限制了反应动力学和H2O2的产率.在这一工作中我们通过将模型催化剂Pt-TiO2沉积在疏水多孔碳基底上,构建了具有气液固三相界面微环境的催化体系.基于这种三相体系,O2能够从空气中快速输送至反应界面,从而大大提高其在反应区的浓度.与传统的固液两相催化体系相比,三相体系中的H2O2的生成速率常数提高了 10倍以上.这项工作突出了反应界面调控对催化反应性能的重要影响,为开发高效H2O2合成体系提供了思路.
Abstract
The two-electron oxygen reduction driven by formic acid based on metal catalysts is a promising approach for H2O2 synthesis under mild conditions.However,in con-ventional catalytic systems,the concentration of reactant O2 at the solid/liquid diphase reaction interface is generally low,which restricts the reaction kinetics and the yield of H2O2.Inspired by the natural non-wetting surfaces,we describe here a catalytic system with an air-liquid-solid triphase interface microenvironment for efficient H2O2 generation in formic acid-driven oxygen reduction.The triphase system was fabri-cated by immobilizing Pt-decorated TiO2(Pt-TiO2),a model catalyst on a hydrophobic porous carbon substrate.Such a triphase system allows sufficient O2 to be rapidly delivered from the air phase,greatly enhancing its concentration at the reaction zone.We found the H2O2 formation rate constant was increased by more than 10-fold in comparison with a con-ventional solid/liquid diphase catalytic system.In addition,the design principle is applicable to a wide range of catalysts.This work provides an exploratory platform for the further development of high-efficiency H2O2 generation systems.
关键词
H2O2 synthesis/HCOOH-driven oxygen reduction/triphase interface microenvironment/Pt-TiO2Key words
H2O2 synthesis/HCOOH-driven oxygen reduction/triphase interface microenvironment/Pt-TiO2引用本文复制引用
基金项目
National Key R&D Program of China(2019YFA0709200)
National Natural Science Foundation of China(21988102)
National Natural Science Foundation of China(51772198)
National Natural Science Foundation of China(21975171)
Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)()
出版年
2024
NETL
NSTL
万方数据