近日，中国科学院大连化学物理研究所杨冰团队研究了催化多米诺效应：反应网络与催化剂重构的一致性加速CO₂加氢表面渗碳。2025年5月29日，《美国化学会志》发表了这一成果。

动态渗碳是许多工业反应中常见且重要的现象。找到控制这一过程的关键因素对于催化剂优化具有重要意义，由于催化剂动力学和反应动力学之间的一致性，催化剂优化变得复杂。在这项工作中，研究组通过揭示长期CO₂加氢反应中反应网络和催化剂重组之间的多米诺骨牌效应，操纵了Pd-FeO_x表面快速渗碳的原位形成。

研究组制备了三种尺寸的催化剂（5Pd-FeO_x、0.5Pd-FeO_x和0.05Pd-FeO_x），发现大尺寸的Pd-NP（5Pd-FeO_x）诱导了反应性金属-载体相互作用，随后是原位Pd₃Fe形成、反应路线改变、快速表面渗碳（Fe₅C₂），最后是优异的催化性能。

在这些变化中，研究组发现原位合金化而不是表观尺寸差异对活性Fe₅C₂相的形成至关重要。作为概念验证，他们进一步设计了一种在FeO_x上预合成的Pd₃Fe合金，并发现通过控制快速渗碳可以提高活性，减少Pd负载。这项工作不仅证明了动态渗碳的可控性，而且通过全面了解原位催化剂的变化，为优化催化剂提供了基准。

附：英文原文 

Title: Domino Effect of Catalysis: Coherence between Reaction Network and Catalyst Restructuring Accelerating Surface Carburization for CO2 Hydrogenation

Author: Pengfei Du, Yafeng Zhang, Rui Qi, Qingqing Gu, Xiaoyan Xu, Aiqin Wang, Beien Zhu, Bing Yang, Tao Zhang

Issue&Volume: May 29, 2025

Abstract: Dynamic carburization is a common and important phenomenon in many industrial reactions. Finding the critical factor governing this process is significant for catalyst optimization, which is complicated due to the coherence between catalyst dynamics and reaction dynamics. In this work, we manipulate the in situ formation of fast carburization on the Pd-FeOx surface by revealing a domino effect between the reaction network and catalyst restructuring during long-term CO2 hydrogenation reaction. We prepared catalysts of three sizes  (5Pd-FeOx, 0.5Pd-FeOx, 0.05Pd-FeOx) and found that the large size of Pd NP (5Pd-FeOx) induces the reactive metal–support interaction, following the in situ Pd3Fe formation, the reaction route change, the fast surface carburization (Fe5C2), and finally the superior catalytic performance. Among these changes, we identify that in situ alloying instead of the apparent size difference is crucial for the formation of the active Fe5C2 phase. As a proof of concept, we further design a presynthesized Pd3Fe alloy on FeOx and find an enhanced activity with reduced Pd loading by controlled fast carburization. This work not only demonstrates the controllability of dynamic carburization but also presents a benchmark of optimizing catalysts through the comprehensive understanding of in situ catalyst changes.

DOI: 10.1021/jacs.5c01435

Source: https://pubs.acs.org/doi/abs/10.1021/jacs.5c01435