Contribution of Carbon Clusters to Ammonia Synthesis Over Ru-Based Catalysts - Details

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Abstract：

Ammonia　(NH3)　plays　an　important　role　in　the　development　and　evolution　of　Earth＇s　life　system.　The　extremely　high　bond　energy　(941 kJ　mol−1)　of　N2　hinder　the　conversion　of　N2　to　NH3　under　mild　conditions.　Meanwhile,　clearly　identifying　the　distribution　of　intermediates　for　NH3　synthesis　remains　a　huge　challenge　in　the　experiment.　Herein,　we　anchored　carbon　clusters　(C60　or　C70)　onto　Ru　catalysts　supported　on　rare　earth　oxides,　forming　a　class　of　Ru-carbon　cluster　co-catalysts　that　exhibit　strong　electronic　metal-carbon　cluster　interaction　(EMCI).　Carbon　clusters　function　as　an　electron　buffer　that　induced　electron　uptake　from　metallic　Ru　sites　and　concurrently　provides　electron　feedback　to　Ruδ+　in　a　reversible　manner,　achieving　a　flexible　balance　of　electron　density　at　the　Ru　active　sites.　Moreover,　H-affinitive　carbon　clusters　serve　as　the　site　for　the　adsorption,　activation　and　migration　of　hydrogen.　With　Ru　and　carbon　clusters　synergistically　bridged　by　hydrogen　spillover,　the　Ru-C60　co-catalyst　exhibits　an　exceptionally　high　NH3　synthesis　rate　and　remarkable　stability.　Experimental　provides　direct　evidence　of　the　distribution　and　evolution　of　*N2Hx　(x　=　1∼3)　intermediates,　with　the　hydrogenation　of　*NH2　to　form　*NH3　identified　as　the　rate-determining　step.　This　work　paves　the　way　for　utilizing　carbon　clusters　in　important　chemical　reactions.　©　2024　Wiley-VCH　GmbH.

Keyword：

Ammonia Hydrogenation Reaction intermediates Ruthenium compounds

Community：

[ 1 ] [Zhang, Mingyuan]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fujian, Fuzhou; 350002, China
[ 2 ] [Zhang, Mingyuan]Qingyuan Innovation Laboratory, Fujian, Quanzhou; 362801, China
[ 3 ] [Luo, Yongjin]College of Environmental and Resource Sciences, College of Carbon Neutral Modern Industry, Fujian Normal University, Fuzhou; 350007, China
[ 4 ] [Peng, Xuanbei]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fujian, Fuzhou; 350002, China
[ 5 ] [Peng, Xuanbei]Qingyuan Innovation Laboratory, Fujian, Quanzhou; 362801, China
[ 6 ] [Zhang, Shiyong]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fujian, Fuzhou; 350002, China
[ 7 ] [Zhang, Lei]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fujian, Fuzhou; 350002, China
[ 8 ] [Xu, Cong-Qiao]Department of Chemistry and Guangdong Provincial Key Laboratory of Catalytic Chemistry, Southern University of Science and Technology, Shenzhen; 518055, China
[ 9 ] [Zhou, Yanliang]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fujian, Fuzhou; 350002, China
[ 10 ] [Zheng, Lirong]Institute of High Energy Physics, Chinese Academy of Sciences, Beijing; 100049, China
[ 11 ] [Ni, Jun]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fujian, Fuzhou; 350002, China
[ 12 ] [Wang, Xiuyun]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fujian, Fuzhou; 350002, China
[ 13 ] [Wang, Xiuyun]Qingyuan Innovation Laboratory, Fujian, Quanzhou; 362801, China
[ 14 ] [Jiang, Lilong]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fujian, Fuzhou; 350002, China
[ 15 ] [Jiang, Lilong]Qingyuan Innovation Laboratory, Fujian, Quanzhou; 362801, China
[ 16 ] [Li, Jun]Department of Chemistry and Engineering Research Center of Advanced Rare-Earth Materials of Ministry of Education, Tsinghua University, Beijing; 100084, China

Reprint 's Address：

[xu, cong-qiao]department of chemistry and guangdong provincial key laboratory of catalytic chemistry, southern university of science and technology, shenzhen; 518055, china;;

Email：

xywang2017@fzu.edu.cnxucq@sustech.edu.cn

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Classification

202.7.1.5 Ruthenium and Alloys - 802.2 Chemical Reactions - 804 Chemical Products - 804.2 Inorganic Compounds

Type

M.Z.　and　Y.L.　contributed　equally　to　this　work.　The　work　was　supported　by　the　National　Key　Research　and　Development　Program　of　China　(2022YFA1604101,　2022YFA1503900,　and　2023YFA1506600),　the　National　Natural　Science　Foundation　of　China　(22222801,　92361303,　22038002,　22478075,　22472028,　22478072,　22108037,　22033005,　and　22103035),　the　NSFC　Center　for　Single-Atom　Catalysis　(22388102),　and　partially　sponsored　by　the　Guangdong　Provincial　Key　Laboratory　Of　Catalysis　(No.　2020B121201002).　Computational　resources　were　supported　by　the　Center　for　Computational　Science　and　Engineering　at　Southern　University　of　Science　and　Technology,　CHEM　high-performance　supercomputer　cluster　(CHEM-HPC)　and　Tsinghua　National　Laboratory　for　Information　Science　and　Technology.M.Z.　and　Y.L.　contributed　equally　to　this　work.　The　work　was　supported　by　the　National　Key　Research　and　Development　Program　of　China　(2022YFA1604101,　2022YFA1503900,　and　2023YFA1506600),　the　National　Natural　Science　Foundation　of　China　(22222801,　92361303,　22038002,　22478075,　22472028,　22478072,　22108037,　22033005,　and　22103035),　the　NSFC　Center　for　Single‐Atom　Catalysis　(22388102),　and　partially　sponsored　by　the　Guangdong　Provincial　Key　Laboratory　Of　Catalysis　(No.　2020B121201002).　Computational　resources　were　supported　by　the　Center　for　Computational　Science　and　Engineering　at　Southern　University　of　Science　and　Technology,　CHEM　high‐performance　supercomputer　cluster　(CHEM‐HPC)　and　Tsinghua　National　Laboratory　for　Information　Science　and　Technology.

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Project No.

Access Number

EI:20244917481350

Language

English

Corresponding s email

xywang2017@fzu.edu.cnxucq@sustech.edu.cn

Author Info

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Source ：

Advanced Functional Materials

ISSN： 1616-301X

Year： 2025

Issue： 8

Volume： 35

1 8 . 5 0 0

JCR@2023

CAS Journal Grade：1

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30 Days PV： 0

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