物理化学学报 >> 2026, Vol. 42 >> Issue (11): 100367.doi: 10.1016/j.actphy.2026.100367

论文 上一篇    

二维Ta2C助催化剂用于增强光催化H2O2合成及有机污染物降解

何琳1, 陈林1, 陈润东1, 周贤龙2, 张帅3, 夏兵全1,4   

  1. 1 武汉工程大学化学与环境工程学院, 磷矿及其共伴生资源绿色高效开发利用全国重点实验室, 湖北 武汉 430074;
    2 南京林业大学化学工程学院, 江苏省林业资源高效加工利用协同创新中心, 江苏 南京 210037;
    3 School of Chemical Engineering, Adelaide University, Adelaide 5005, South Australia, Australia;
    4 Schulich School of Engineering, University of Calgary, Calgary T2N 1N4, Alberta, Canada
  • 收稿日期:2026-06-12 修回日期:2026-07-11 录用日期:2026-07-12 发布日期:2026-09-29
  • 通讯作者: 张帅, 夏兵全 E-mail:shuai.zhang02@adelaide.edu.au;xiab@wit.edu.cn
  • 基金资助:
    本研究得到了国家自然科学基金(22409151, 22402083);国家留学基金委;武汉工程大学科学基金(23QD02)以及武汉工程大学研究生创新基金(CX2025140)的资助。

Two-dimensional Ta2C cocatalyst for enhanced H2O2 photosynthesis and organic pollutant degradation

Lin He1, Lin Chen1, Rundong Chen1, Xianlong Zhou2, Shuai Zhang3, Bingquan Xia1,4   

  1. 1 State Key Laboratory of Green and Efficient Development of Phosphorus Resources, School of Chemistry and Environmental Engineering, Wuhan Institute of Technology, Wuhan 430074, Hubei Province, China;
    2 Jiangsu Co-Innovation Centre of Efficient Processing and Utilization of Forest Resources, College of Chemical Engineering, Nanjing Forestry University, Nanjing 210037, Jiangsu Province, China;
    3 School of Chemical Engineering, Adelaide University, Adelaide 5005, South Australia, Australia;
    4 Schulich School of Engineering, University of Calgary, Calgary T2N 1N4, Alberta, Canada
  • Received:2026-06-12 Revised:2026-07-11 Accepted:2026-07-12 Published:2026-09-29
  • Contact: Shuai Zhang, Bingquan Xia E-mail:shuai.zhang02@adelaide.edu.au;xiab@wit.edu.cn

摘要: 过氧化氢(H2O2)作为一种环境友好型氧化剂,其光催化合成与环境修复相结合是一种极具吸引力的策略。为解决传统光催化剂中电荷动力学缓慢和表面反应受限的问题,本研究探索了二维碳化钽(Ta2C) MXene作为有效助催化剂,用于调控石墨相氮化碳(g-C3N4)的界面电子结构,从而实现高效H2O2制备以及盐酸四环素(TCH)的降解。系统表征和理论计算表明,两种组分之间显著的功函数差异诱导费米能级平衡,并促进内建电场的形成,从而驱动光生电子从g-C3N4定向迁移至Ta2C,加速电荷分离并抑制电荷复合。优化后的g-C3N4/Ta2C-6 (CT-6)复合材料实现了4584.7 μmol g-1 h-1的H2O2产率,并在1 h内降解了86.56%的TCH,显著优于原始g-C3N4。机理研究表明,H2O2主要通过两步单电子氧还原途径生成,反应中产生的活性氧物种在TCH降解中起关键作用。本研究证明了Ta2C作为非贵金属助催化剂的潜力,并建立了MXene基异质结中界面电子结构、电荷转移动力学与光催化反应途径之间的明确关联,为设计高性能、多功能光催化剂提供了原子层面的见解和理论基础。

关键词: H2O2制备, 石墨相氮化碳, Ta2C MXene, 助催化剂

Abstract: Hydrogen peroxide (H2O2) serves as an environmentally benign oxidant, and its photocatalytic synthesis coupled with environmental remediation is an extremely attractive strategy. To address sluggish charge dynamics and surface reaction in conventional photocatalysts, two-dimensional tantalum carbide (Ta2C) MXene was explored as an effective cocatalyst to engineer the interfacial electronic structure of graphitic carbon nitride (g-C3N4), enabling highly efficient H2O2 production and simultaneous tetracycline hydrochloride (TCH) degradation. Systematic characterization and theoretical calculations revealed that the significant work function difference between the two components induces Fermi level equilibration and facilitates built-in electric field formation, which drives directional photogenerated electron migration from g-C3N4 to Ta2C, accelerating charge separation and suppressing charge recombination. The optimized g-C3N4/Ta2C-6 (CT-6) composite achieved an H2O2 production rate of 4584.7 μmol g-1 h-1, together with 86.56% of TCH degradation within 1 h, markedly outperforming pristine g-C3N4. Mechanistic studies show that H2O2 is mainly produced through a two-step one-electron oxygen reduction pathway, and the reactive oxygen species generated in the reaction play a key role in TCH degradation. This study demonstrates the potential of Ta2C as a non-noble-metal cocatalyst and establishes a clear correlation between interfacial electronic structure, charge transfer dynamics and photocatalytic reaction pathways in MXene-based heterojunctions, offering atomic-level insights and theoretical basis for the design of high-performance, multifunctional photocatalysts.

Key words: H2O2production, Graphitic carbon nitride, Ta2C MXene, Cocatalyst