近日，美国西北大学Joseph T. Hupp团队实现了孤立H₂还原的安德森型簇催化CO₂低温加氢制甲醇。2026年3月23日出版的《自然-化学》杂志发表了这项成果。

二氧化碳加氢，特别是转化为甲醇的反应，对于构建可持续的碳利用闭环系统至关重要。然而，低温下CO₂活化的困难以及构效关系的模糊性，成为降低该加氢过程能耗的阻碍。

研究组报道了定位于坚固金属有机框架内的分子级安德森型PtMo₆O₂₄簇合物，可催化低温二氧化碳加氢反应。该簇合物在180°C下运行3600小时，其活性和甲醇选择性均未显现衰减迹象，且在相似条件下，其单程产率超越了现有非均相催化剂的水平。结合原位光谱与密度泛函理论计算表明，CH₃OH的生成主要由逆水煤气变换及随后的CO加氢路径主导，而HCOO路径可能作为补充途径。这种结构明确的簇合物为阐明构效关系提供了理想模型，并为理性设计高活性、低温二氧化碳加氢催化剂开辟了激动人心的新途径。

附：英文原文

Title: Isolated and H2-reduced Anderson clusters catalyse low-temperature hydrogenation of CO2 to methanol

Author: Liu, Qin, Rabbani, S. M. Gulam, Hou, Zhenhao, Chen, Zhihengyu, Yang, Haofan, Bi, Wentuan, Chapman, Karena W., Getman, Rachel B., Hupp, Joseph T.

Issue&Volume: 2026-03-23

Abstract: CO2 hydrogenation, especially to methanol, is crucial to establishing sustainable closed-loop systems for carbon utilization. However, the difficulties of CO2 activation at low temperatures and the ambiguity of structure–activity correlations are obstacles to reducing the energy consumption of the hydrogenation process. Here we report that molecularly defined Anderson PtMo6O24 clusters, sited within a robust metal–organic framework, are catalytic for low-temperature CO2 hydrogenation. The performance of the cluster showed no signs of decay in either its activity or methanol selectivity over 3,600h at 180°C. It also achieves a per-pass yield exceeding that of state-of-the-art heterogeneous catalysts under similar conditions. Combined in situ spectroscopy and density functional theory calculations demonstrated that CH3OH formation is dominated by the reverse water–gas shift and subsequent CO* hydrogenation pathway, while the HCOO* pathway may serve as a supplementary route. The well-defined cluster structure offers an ideal model for elucidating structure–activity correlations and opens exciting avenues for the rational design of high-activity, low-temperature catalysts for CO2 hydrogenation.

DOI: 10.1038/s41557-026-02104-x

Source: https://www.nature.com/articles/s41557-026-02104-x