高等学校化学学报

高等学校化学学报

• 研究论文 • 上一篇    下一篇

钛网负载铂枝晶高效电催化丁二烯选择性加氢性能研究

管泽龙1，李子丹1，罗皓文1，王婉仪2，黄传峰2，苏宝连1,3，王朝1   

  1. 1.武汉理工大学材料复合新技术国家重点实验室

    2. 武汉理工大学化学化工与生命科学学院 3.那慕尔大学无机材料化学实验室

  • 收稿日期:2025-11-07 修回日期:2025-12-10 网络首发:2025-12-16 发布日期:2025-12-16
  • 通讯作者: 王朝 E-mail:zhao.wang@whut.edu.cn
  • 基金资助:
    国家自然科学基金（批准号：22293022）和武汉市黄鹤英才计划项目（批准号：202501jc0252）资助

Electrocatalytic Butadiene Selective Hydrogenation over Platinum Dendrite Surfaces on Ti mesh

GUAN Zelong1，LI Zidan1, LUO Haowen1, WANG Wanyi2, HUANG Chuanfeng2, SU Baolian1,3, WANG Zhao1   

  1. 1. Wuhan University of Technology, State Key Laboratory of Advanced Technology for Materials, Synthesis and Processing

    2. Wuhan University of Technology, School of Chemistry 3. Laboratory of Inorganic Materials Chemistry(CMI), University of Namur

  • Received:2025-11-07 Revised:2025-12-10 Online First:2025-12-16 Published:2025-12-16
  • Contact: Zhao Wang E-mail:zhao.wang@whut.edu.cn
  • Supported by:
    Supported by the National Natural Science Foundation of China(No. 22293022) and the “Wuhan Yingcai” Program, China(No. 202501jc0252)

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摘要： 本研究通过控制电沉积时间（x），在钛网表面构筑了具有树突状枝晶铂催化剂（Ptx/Ti），并以水为活性氢[H]源，实现了对单烯烃大宗化学品中二烯烃杂质的高效清洁电催化选择性加氢，重点探究其在低电流密度区间的催化性能及反应机制。性能测试结果表明：当电流密度为-6.25 mA?cm-2时，Pt1200s/Ti电极表现最优，丁二烯转化率达73 %，目标产物法拉第效率超75 %，且连续反应8 h后性能衰减低于3 %。反应动力学解析揭示了铂枝晶表面丁二烯选择性加氢反应机理：低电流密度（0 ~ 6.25 mA·cm-2）下，丁二烯优先吸附并与[H]结合生成丁烯；中电流密度（6.25 ~ 10 mA·cm-2）下，过量[H]推动反应向丁烯过度加氢偏移，导致选择性下降；高电流密度下，过量[H]耦合生成H?，显著降低法拉第效率。本研究为设计高稳定性、高选择性的烯烃加氢电催化剂提供了新思路。

关键词: 丁二烯, 选择性加氢, 铂枝晶电极, 电催化, 电沉积

Abstract: In this study, titanium mesh supported dendritic platinum (Pt) branch catalyst (Ptx/Ti ) was synthesized by an in situ electrodeposition method for the efficient butadiene selective hydrogenation, which is driven by electricity with water as the source of intermediate hydrogen [H]. It shows that the Pt/Ti with 1200s of electrodeposition (Pt1200s/Ti) has a superior performance at a current density of -6.25 mA·cm-2, reaching a butadiene conversion rate of 73 % and a target product Faraday efficiency exceeding 75 % after 8 hours of time on stream. Further analysis reveals that, at current density below 6.25 mA·cm-2, butadiene preferentially adsorbs and reacts with the [H] to form butene with high selectivity; With an increase of current density to 6.25 ~ 10 mA·cm-2, the excessive [H] drives the reaction toward over-hydrogenation of butene, leading to decreased selectivity; Moreover, at current density above 10 mA·cm-2, partial [H] atoms are combined to H? gas, leading to a significant decrease in the Faraday efficiency. This study provides a direction for designing highly stable, selective olefin hydrogenation electrodes.

Key words: Butadiene, Selective hydrogenation, Platinum dendritic electrode, Electro-catalysis, Electrodeposition

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