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具有纳米至埃级精度的铂基金属间化合物的管内配位工程。

Coordination-in-pipe engineering of Pt-based intermetallic compounds with nanometer to angstrom precision.

作者信息

Hu Shouyao, Gong Jiaxin, Tao Yu, Ma Runze, Guan Jianping, Liu Xu, Hu Jinhua, Yan Jun, Wang Shibin, Zhang Zedong, Liang Xiao, Zhuang Zechao, Han Yunhu, Zheng Xusheng, Yan Wensheng, Chen Chengjin, Zhu Wei, Wang Dingsheng, Xiong Yu

机构信息

Department of Chemistry and Chemical Engineering, Central South University Changsha 410083 China

College of Chemical Engineering, Zhejiang University of Technology Hangzhou 310032 China.

出版信息

Chem Sci. 2025 Jan 27;16(10):4311-4319. doi: 10.1039/d4sc07905a. eCollection 2025 Mar 5.

DOI:10.1039/d4sc07905a
PMID:39911330
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11791777/
Abstract

The simultaneous regulation of particle size, surface coordinated environment and composition for Pt-based intermetallic compound (Pt-IMC) nanoparticles to manipulate their reactivity for energy storage is of great importance. Herein, we report a general synthetic method for Pt-IMCs using SBA-15 for coordination-in-pipe engineering. The particle size can be regulated to 3-9 nm by carrying out the coordination in pipes with different diameters and the coordination number of the interface metal atoms can be adjusted by altering the N source. Moreover, this strategy can also be expanded to the synthesis of Pt-IMCs with the majority of fourth period transition metals (Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn). The PtCo IMC using 1,10-phenanthroline as the nitrogen source (PtCo@CN) shows the highest catalytic performance in the methanol oxidation reaction (MOR; 2.19 A mg ) among the investigated nitrogen sources. The high chemical states of surface Pt and Co, affected by the nitrogen coordination number at the angstrom scale, facilitate electron accumulation on active sites, reduce the activation energy of the rate-determining step and enhance the catalytic performance of Pt-IMCs in the MOR.

摘要

同时调控基于铂的金属间化合物(Pt-IMC)纳米颗粒的粒径、表面配位环境和组成,以调控其用于能量存储的反应活性具有重要意义。在此,我们报道了一种使用SBA-15进行管内配位工程的通用合成Pt-IMC的方法。通过在不同直径的管内进行配位,粒径可调控至3-9 nm,并且通过改变氮源可调节界面金属原子的配位数。此外,该策略还可扩展至合成含有大多数第四周期过渡金属(Ti、V、Cr、Mn、Fe、Co、Ni、Cu、Zn)的Pt-IMC。在所研究的氮源中,使用1,10-菲咯啉作为氮源的PtCo IMC(PtCo@CN)在甲醇氧化反应(MOR;2.19 A mg)中表现出最高的催化性能。受埃尺度氮配位数影响的表面Pt和Co的高化学态,促进了活性位点上的电子积累,降低了速率决定步骤的活化能,并提高了Pt-IMC在MOR中的催化性能。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/52df/11881228/4f67b803a302/d4sc07905a-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/52df/11881228/741be41b753b/d4sc07905a-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/52df/11881228/aa7be1443a6c/d4sc07905a-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/52df/11881228/cdd215f9d0f2/d4sc07905a-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/52df/11881228/6015236998d6/d4sc07905a-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/52df/11881228/4f67b803a302/d4sc07905a-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/52df/11881228/741be41b753b/d4sc07905a-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/52df/11881228/aa7be1443a6c/d4sc07905a-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/52df/11881228/cdd215f9d0f2/d4sc07905a-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/52df/11881228/6015236998d6/d4sc07905a-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/52df/11881228/4f67b803a302/d4sc07905a-f5.jpg

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