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金属-O-Fe键的环境可在单个金属原子和负载纳米颗粒上实现高活性CO2还原
作者:小柯机器人 发布时间:2021/4/7 13:32:37

美国西北太平洋国家实验室Oliver Y. Gutiérrez团队报道了金属-O-Fe键的环境可在单个金属原子和负载纳米颗粒上实现高活性CO2还原。 相关研究成果于2021年4月5日发表在国际知名学术期刊《美国化学会杂志》。

据报道,单原子催化剂的催化性能往往超过纳米颗粒,但缺乏对两者的共同点和不同点的直接比较。

该文中,研究人员发现嵌入Fe3O4表面的Pt族金属的单原子与CO2的相互作用强度比Fe3O4表面大得多。单个Rh原子对CO2的强吸附和相应的低活化能使CO2的转化率比Rh纳米粒子高2个数量级。单原子的这种高活性源于其与载体的配位所产生的部分氧化状态。Fe3O4负载Rh纳米粒子在CO2相互作用和还原过程中遵循单原子行为,这是由于Fe3O4-Rh界面上部分氧化位点的主导作用。

因此,研究人员展示了两种被认为是不同的材料的一种可能共同的催化化学,并且展示了Pt族金属在Fe3O4上的单原子,对于主要依赖于金属–O–Fe环境的位点的催化反应是特别成功的材料。

附:英文原文

Title: Environment of Metal–O–Fe Bonds Enabling High Activity in CO2 Reduction on Single Metal Atoms and on Supported Nanoparticles

Author: Yifeng Zhu, Simuck F. Yuk, Jian Zheng, Manh-Thuong Nguyen, Mal-Soon Lee, Janos Szanyi, Libor Kovarik, Zihua Zhu, Mahalingam Balasubramanian, Vassiliki-Alexandra Glezakou, John L. Fulton, Johannes A. Lercher, Roger Rousseau, Oliver Y. Gutiérrez

Issue&Volume: April 5, 2021

Abstract: Single-atom catalysts are often reported to have catalytic properties that surpass those of nanoparticles, while a direct comparison of sites common and different for both is lacking. Here we show that single atoms of Pt-group metals embedded into the surface of Fe3O4 have a greatly enhanced interaction strength with CO2 compared with the Fe3O4 surface. The strong CO2 adsorption on single Rh atoms and corresponding low activation energies lead to 2 orders of magnitude higher conversion rates of CO2 compared to Rh nanoparticles. This high activity of single atoms stems from the partially oxidic state imposed by their coordination to the support. Fe3O4-supported Rh nanoparticles follow the behavior of single atoms for CO2 interaction and reduction, which is attributed to the dominating role of partially oxidic sites at the Fe3O4–Rh interface. Thus, we show a likely common catalytic chemistry for two kinds of materials thought to be different, and we show that single atoms of Pt-group metals on Fe3O4 are especially successful materials for catalyzed reactions that depend primarily upon sites with the metal–O–Fe environment.

DOI: 10.1021/jacs.1c02276

Source: https://pubs.acs.org/doi/10.1021/jacs.1c02276

 

期刊信息

JACS:《美国化学会志》,创刊于1879年。隶属于美国化学会,最新IF:14.612
官方网址:https://pubs.acs.org/journal/jacsat
投稿链接:https://acsparagonplus.acs.org/psweb/loginForm?code=1000