Coupling metal and support clusters dictates the reactivity of Ru catalysts for ammonia synthesis

IF 4.3 2区工程技术 Q2 ENGINEERING, CHEMICAL Chemical Engineering Science Pub Date : 2025-06-15 Epub Date: 2025-04-18 DOI:10.1016/j.ces.2025.121676

Tianhua Zhang , Yangyu Zhang , Zuo-Chang Chen , Yujue Qiu , Mingyuan Zhang , Shiyong Zhang , Xuanbei Peng , Lei Zhang , Yanliang Zhou , Lirong Zheng , Bo-Qing Xu , Xiuyun Wang , Lilong Jiang

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Abstract

Strong metal-support interaction (SMSI) is a crucial strategy for modulating the activity. Finely tailoring the size of the support to the nanoscale still faces significant challenges. Herein, for the first time, C₆₀ carbon cluster is utilized as a nano-support to anchor ultrafine Ru nanoclusters to create a Ru-C₆₀ cluster–cluster co-catalyst. The unique geometric structure of the nano-support C₆₀ enables the construction of a strong cluster–cluster interaction (SCCI), quite different from traditional SMSI. La-modified Ru-C₆₀ presents a surprising discovery that NH₃ can even be synthesized at 150 °C, and exhibits an unprecedentedly high NH₃ synthesis rate at 400 °C. C₆₀ not only acts as an electron buffer to balance the charge density of Ru sites, but also stabilizes more metallic Ru active sites with a smaller size due to its spatial and SCCI effect, thereby achieving superior catalytic performance over a wide range of temperatures and pressures.

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偶联金属和支撑团簇决定了Ru催化剂合成氨的反应活性

强金属-支撑相互作用（SMSI）是调节活性的关键策略。将支架的尺寸精确地调整到纳米级仍然面临着重大挑战。本文首次利用C60碳团簇作为纳米载体，锚定超细Ru纳米团簇，制备Ru-C60团簇-团簇共催化剂。纳米支撑C60独特的几何结构使其能够构建强的簇-簇相互作用（SCCI），这与传统的SMSI完全不同。la修饰的Ru-C60惊人地发现在150 °C下也能合成NH3，并在400 °C下表现出前所未有的高NH3合成速率。C60不仅可以作为电子缓冲器平衡Ru位点的电荷密度，而且由于其空间和SCCI效应，可以稳定更多较小尺寸的金属Ru活性位点，从而在较宽的温度和压力范围内获得优异的催化性能。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Chemical Engineering Science 工程技术-工程：化工

CiteScore

7.50

自引率

8.50%

发文量

1025

审稿时长

50 days

期刊介绍： Chemical engineering enables the transformation of natural resources and energy into useful products for society. It draws on and applies natural sciences, mathematics and economics, and has developed fundamental engineering science that underpins the discipline. Chemical Engineering Science (CES) has been publishing papers on the fundamentals of chemical engineering since 1951. CES is the platform where the most significant advances in the discipline have ever since been published. Chemical Engineering Science has accompanied and sustained chemical engineering through its development into the vibrant and broad scientific discipline it is today.