课题基金基金详情
室内甲醛催化氧化过程中关键中间体(CH2OO)的特征反应性研究
结题报告
批准号:
22006071
项目类别:
青年科学基金项目
资助金额:
24.0 万元
负责人:
李海玮
依托单位:
学科分类:
大气污染与控制化学
结题年份:
2023
批准年份:
2020
项目状态:
已结题
项目参与者:
李海玮
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中文摘要
我国室内甲醛污染形势依然严峻,居民对甲醛污染的投诉仍高发频发。以常温催化氧化为核心的主动控制技术实现了在较低室温下消除甲醛。然而,甲醛氧化降解过程极具反复性,这归因于关键中间体甲醛氧化物(CH2OO)的形成转化,其存在多种同分异构体且在不同湿度下呈现出复杂的化学反应性,造成CH2OO的反应壁垒高于甲醛一次氧化。由于催化反应致使CH2OO反应速率更快和环境寿命更短,故针对其的直接测定极具困难,导致甲醛完全氧化路径和机制的研究很不充分,往往通过理论计算进行推测。本项目将率先利用步进扫描时间分辨傅里叶变换红外光谱在线测定甲醛催化氧化中CH2OO的化学组成和研究温、湿度变化对其生成、稳定和衰变的反应性的影响,旨在对现有甲醛污染研究和治理形成重要的补充和推进。本项目将以“研反应-优设计”为导向,通过阐明CH2OO关键中间体反应特征为设计优化高效甲醛催化体系提供策略支撑,致力于提升室内空气质量。
英文摘要
The situation of formaldehyde (HCHO) pollution in indoors is still severe in China, and the most common complaints are frequently reported in occupational HCHO exposures. Room-temperature catalytic oxidation (RCO) has become a promising approach to remove HCHO in indoor air at low room temperatures. Although HCHO has the simplest molecular composition, the complete catalytic oxidation of HCHO cannot accomplish in an action. This limitation is mostly ascribed by the production of key intermediates, namely, formaldehyde oxides (CH2OO), which have complicated and reactive isomers under various moisture levels. The ensuing conversion from CH2OO intermediates becomes more complex and difficult than that from HCHO initially. To date, making direct measurements of CH2OO intermediates in the oxidation of HCHO is challenging, instead they are roughly estimated by theoretical calculation, as they are quite reactive and have extremely short lifetime. Herein, we will make an interesting contribution to unveil the chemical speciation and reactivity of CH2OO in the HCHO catalytic oxidation using step scan time-resolved Fourier transform infrared spectroscopy for the first time, and to investigate the effects of ambient temperatures and moistures on the formation, stabilization, and decay of the CH2OO isomers. This proposed project will fill the knowledge gap in scientific research and formulating mitigation strategy for the HCHO removal. Most importantly, this project is expected to attain a research outline of probing chemical reaction towards optimizing catalyst design, as of determining the complete reactivity mechanisms and pathways of HCHO and CH2OO intermediates to provide strategic insights into rational design and CO2 selectivity enhancement of a reliable catalytic oxidation process for the improvement of indoor air quality.
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DOI:https://doi.org/10.1016/j.envres.2022.113064
发表时间:2022
期刊:Environmental Research
影响因子:--
作者:Yuan Wang;Shijie Cui;Xuewei Fu;Yunjiang Zhang;Junfeng Wang;Pingqing Fu;Xinlei Ge;Haiwei Li;Xinming Wang
通讯作者:Xinming Wang
DOI:10.3390/toxics12010034
发表时间:2024-01-01
期刊:Toxics
影响因子:4.6
作者:Cao L;Men Q;Zhang Z;Yue H;Cui S;Huang X;Zhang Y;Wang J;Chen M;Li H
通讯作者:Li H
DOI:10.1016/j.chemosphere.2023.138185
发表时间:2023-02
期刊:Chemosphere
影响因子:8.8
作者:Haiwei Li;L. Cui;Yu Huang;Yunjiang Zhang;Junfeng Wang;Mindong Chen;X. Ge
通讯作者:Haiwei Li;L. Cui;Yu Huang;Yunjiang Zhang;Junfeng Wang;Mindong Chen;X. Ge
DOI:10.1007/s40726-023-00287-2
发表时间:2024-01
期刊:Current Pollution Reports
影响因子:7.3
作者:Zihao Zhang;Haiwei Li;Wingkei Ho;Long Cui;Qihui Men;Li Cao;Yunjiang Zhang;Junfeng Wang;Cheng Huang;Shun-cheng Lee;Yu Huang;Mindong Chen;Xinlei Ge
通讯作者:Zihao Zhang;Haiwei Li;Wingkei Ho;Long Cui;Qihui Men;Li Cao;Yunjiang Zhang;Junfeng Wang;Cheng Huang;Shun-cheng Lee;Yu Huang;Mindong Chen;Xinlei Ge
DOI:10.13578/j.cnki.issn.1671-1556.20210042
发表时间:2021
期刊:安全与环境工程
影响因子:--
作者:乐昊;李海玮;盖鑫磊
通讯作者:盖鑫磊
大气中锰纳米颗粒物表界面介导的氧自由基形成与非均相化学反应研究
  • 批准号:
    22376103
  • 项目类别:
    面上项目
  • 资助金额:
    50.00万元
  • 批准年份:
    2023
  • 负责人:
    李海玮
  • 依托单位:
国内基金
海外基金