由水性钯针组装体催化的一氧化碳加氢制甲酸反应。

CO hydrogenation to HCOOH catalyzed by aqueous Pd needle assembly.

作者信息

Wang Mengjun, Jia Jun, Xia Jing, Peng Chun-Kuo, He Jinxin, Qiu Yueming, He Yuting, Gao Le, Xue Fei, Lin Yan-Gu, Zhan Guowu, Guo Yuzheng, Huang Xiaoqing, Xu Yong

机构信息

i-Lab, Suzhou Institute of Nano-Tech and Nano-Bionics (SINANO), Chinese Academy of Sciences (CAS), Suzhou, China.

State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China.

出版信息

Nat Commun. 2025 Jul 12;16(1):6454. doi: 10.1038/s41467-025-61747-5.

DOI:10.1038/s41467-025-61747-5

PMID:40651946

原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12255681/

Abstract

Carbon dioxide (CO) conversion to liquid fuels has attracted great attention due to the current environmental concerns and energy crisis. However, the selective conversion of CO to target liquids is formidably challenging due to the chemical inertness of CO. We theoretically and experimentally confirm that the bending of Pd-Pd bond can breaks the asymmetric potential well and facilitate CO adsorption. We have successfully synthesized a new class of Pd nanoneedles via a "close edges and open corners" process, with a magic angle of 60 between the main trunk and branch, and realized the selective CO hydrogenation to formic acid (HCOOH) at room temperature in water. Impressively, a HCOOH productivity of ~250 mmol g in 100 h while maintaining HCOOH selectivity over 99%. This work bridges nanostructure design and catalytic application, which may open a new avenue for selective CO conversion in an elegant manner.

摘要

由于当前的环境问题和能源危机，二氧化碳（CO₂）转化为液体燃料备受关注。然而，由于CO₂的化学惰性，将其选择性转化为目标液体极具挑战性。我们通过理论和实验证实，Pd-Pd键的弯曲可以打破不对称势阱并促进CO₂吸附。我们通过“封闭边缘和开放角落”工艺成功合成了一类新型的Pd纳米针，其主干和分支之间的神奇角度为60°，并实现了在室温下于水中将CO₂选择性加氢生成甲酸（HCOOH）。令人印象深刻的是，在100小时内HCOOH的产率约为250 mmol g，同时保持HCOOH的选择性超过99%。这项工作架起了纳米结构设计与催化应用之间的桥梁，可能会以一种巧妙的方式为CO₂的选择性转化开辟一条新途径。