
近日,新加坡国立大学颜宁团队报道了随时间变化的表面极化打破了选择性乙炔加氢的静态结垢关系。2026年4月13日出版的《自然-化学》杂志发表了这项成果。
控制表面-吸附物相互作用对于推动众多化学过程至关重要。化学相关表面物种之间吸附能的静态标度关联限制了化学过程中的选择性,例如多相催化中存在的约束。
研究组证明,在振荡电势下的动态表面极化能够克服钯催化乙炔半加氢反应中的这一限制。与仅能略微提高乙烯选择性的静态极化不同,动态极化在不进一步牺牲转化率的情况下显著提升了选择性,从而获得了高乙烯产率。通过加氢动力学、原位漫反射红外傅里叶变换光谱、X射线吸收光谱和密度泛函理论获得的机理研究表明,时间依赖的极化动态地调控了Pd的电子结构和吸附能量。
在乙炔加氢过程中,极化正偏压时处于强结合态,而在乙烯生成过程中,极化负偏压时切换为弱结合态,这种交替有效地抑制了过度加氢,同时保持了半加氢活性。这项工作确立了动态电表面调控可作为一种解耦吸附能关联的强大策略,以改善多相催化及其他吸附介导的过程。
附:英文原文
Title: Time-dependent surface polarization breaks static scaling relationship for selective acetylene hydrogenation
Author: Xu, Di, Hlsey, Max J., Chen, Chen, Lim, Chia Wei, Chen, Hongqiu, Sun, Geng, Sautet, Philippe, Liu, Zhaolin, Yan, Ning
Issue&Volume: 2026-04-13
Abstract: Controlling the surface-adsorbates interactions is critical to advancing numerous chemical processes. Static scaling correlations between adsorption energies of chemically related surface species impose limits on selectivity in chemical processes, as exemplified by constraints in heterogeneous catalysis. Here we demonstrate that dynamic surface polarization under oscillating electric potentials can overcome this limitation in Pd-catalysed acetylene semi-hydrogenation. Unlike static polarization, which only imparts a minor improvement to ethylene selectivity, dynamic polarization drastically enhances selectivity without further sacrificing conversion, yielding a high ethylene productivity. Mechanistic insights from hydrogenation kinetics, in situ diffuse reflectance infrared Fourier transform spectroscopy, X-ray absorption spectroscopy and density functional theory reveal that time-dependent polarization dynamically modulates the Pd’s electronic structure and adsorption energetics. Alternating between strong-binding states with positive polarization during acetylene hydrogenation and weak-binding states with negative polarization during ethylene formation effectively suppresses over-hydrogenation while maintaining semi-hydrogenation activity. This work establishes dynamic electric surface modulation as a powerful strategy for decoupling adsorption-energy correlations to improve heterogeneous catalysis and other adsorption-mediated processes.
DOI: 10.1038/s41557-026-02107-8
Source: https://www.nature.com/articles/s41557-026-02107-8
Nature Chemistry:《自然—化学》,创刊于2009年。隶属于施普林格·自然出版集团,最新IF:24.274
官方网址:https://www.nature.com/nchem/
投稿链接:https://mts-nchem.nature.com/cgi-bin/main.plex
