形貌调控ZnO晶面对光催化甲烷选择性氧化性能的影响

丁强; 王昊智; 赵越; 陈艳群; 王建成; 左志军

doi:10.11949/0438-1157.20260538

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形貌调控ZnO晶面对光催化甲烷选择性氧化性能的影响

催化、动力学与反应器 | 更新时间：2026-08-14

- 形貌调控ZnO晶面对光催化甲烷选择性氧化性能的影响
- Effect of Morphology Regulated ZnO Facets on the Photocatalytic Selective Oxidation of Methane
- 化工学报 2026年
- 作者机构：
  
  1.太原理工大学环境与生态学院，山西太原 030024
  2.太原理工大学化学与化工学院，山西太原 030024
- 作者简介：
  
  丁强（1982-），男，博士研究生，277568448@qq.com
  王建成（1978-），男，博士，教授，wangjiancheng@tyut.edu.cn
  左志军（1981-），男，博士，教授，zuozhijun@tyut.edu.cn
- 基金信息：
  
  国家自然科学基金项目(U25A20554;U21A20319)
- DOI：10.11949/0438-1157.20260538
  中图分类号： TQ51
- 收稿：2026-04-15，
  
  修回：2026-08-08，
  
  录用：2026-08-14，
- 稿件说明：
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丁强, 王昊智, 赵越, 等. 形貌调控ZnO晶面对光催化甲烷选择性氧化性能的影响[J/OL]. 化工学报, 2026.

Qiang Ding, Haozhi Wang, Yue Zhao, et al. Effect of Morphology Regulated ZnO Facets on the Photocatalytic Selective Oxidation of Methane[J/OL]. CIESC Journal, 2026.
丁强, 王昊智, 赵越, 等. 形貌调控ZnO晶面对光催化甲烷选择性氧化性能的影响[J/OL]. 化工学报, 2026. DOI： 10.11949/0438-1157.20260538.

Qiang Ding, Haozhi Wang, Yue Zhao, et al. Effect of Morphology Regulated ZnO Facets on the Photocatalytic Selective Oxidation of Methane[J/OL]. CIESC Journal, 2026. DOI： 10.11949/0438-1157.20260538.

摘要

为探究ZnO催化剂晶面对光催化甲烷选择性氧化反应路径的影响机制，本研究基于形貌工程策略，通过调控催化剂表面自由基微环境，采用水热法合成了两种不同晶面暴露的ZnO材料：一种是由纳米颗粒组装而成的纳米片状结构（ZnO-NS），主要暴露(100)晶面；另一种为不规则纳米棒（ZnO-NR），主要暴露(101)晶面。实验结果表明，ZnO-NS的液相产物主要为甲醛和甲酸，而ZnO-NR的液相产物除甲醛和甲酸外还生成乙醛。以ZnO-NS为催化

剂时，甲醛产率最高可达13.12 μmol h

-1

，对应的选择性为89.38%；以ZnO-NR为催化剂时，乙醛选择性最高为35.43%，此时乙醛产率为2.74 μmol h

-1

。表征与理论计算结果表明，ZnO-NS表面高浓度的•OH可促进•CH

定向氧化为甲醛，有效抑制C-C偶联路径；而ZnO-NR表面较低的•CH

/•OH浓度比则使部分•CH

发生偶联生成乙醛。本研究从表面自由基反应动力学层面阐明了形貌工程调控甲烷转化选择性的微观机制，为高效光催化甲烷转化催化剂的设计提供了新思路。

Abstract

To investigate the influence mechanism of ZnO facets on the reaction pathway of photocatalytic selective oxidation of methane

this study employed a morphology engineering strategy to regulate the surface radical microenvironment. Two ZnO materials with different exposed crystal facets were synthesized via a hydrothermal method: one is a nanosheet-assembled structure (ZnO-NS) predominantly exposing the (100) facet

and the other is an irregular nanorod structure (ZnO-NR) predominantly exposing the (101) facet. Experimental results show that the liquid-phase products on ZnO-NS are mainly formaldehyde and formic acid

while the liquid-phase products on ZnO-NR are mainly formaldehyde

formic acid and acetaldehyde. The highest formaldehyde production rate on ZnO-NS reaches 13.12 μmol h

-1

with a corresponding selectivity of 89.38%. The highest acetaldehyde selectivity on ZnO-NR reaches 35.43%

with a corresponding production rate of 2.74 μmol h

-1

. Characterization and theoretical calculation results reveal that the relative concentrations of •OH and •CH

are the key factors governing product selectivity. The high concentration of •OH on the ZnO-NS surface promotes the oriented oxidation of •CH

to formaldehyde

effectively suppressing the C-C coupling pathway; in contrast

the lower •CH

/•OH concentration ratio on the ZnO-NR surface allows partial •CH

to undergo coupling to form acetaldehyde. This work elucidates

from the perspective of surface radical reaction kinetics

the microscopic mechanism by which morphology engineering regulates the selectivity of methane conversion

and prov

ides new insights into the rational design of efficient photocatalysts for methane conversion.

关键词

Keywords

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