Multiple reaction pathway on alkaline earth imide supported catalysts for efficient ammonia synthesis

doi:10.1038/s41467-023-42050-7

	Multiple reaction pathway on alkaline earth imide supported catalysts for efficient ammonia synthesis
	Li, Zichuang 1; Lu, Yangfan 2; Li, Jiang 3; Xu, Miao 4; Qi, Yanpeng5,6,7 ; Park, Sang-Won 3; Kitano, Masaaki 3; Hosono, Hideo 3; Chen, Jie-Sheng 1; Ye, Tian-Nan 1
	2023-10-11
发表期刊	NATURE COMMUNICATIONS (IF:14.7[JCR-2023],16.1[5-Year])
EISSN	2041-1723
卷号	14 期号:1
发表状态	已发表
DOI	10.1038/s41467-023-42050-7
摘要	["The tunability of reaction pathways is required for exploring efficient and low cost catalysts for ammonia synthesis. There is an obstacle by the limitations arising from scaling relation for this purpose. Here, we demonstrate that the alkali earth imides (AeNH) combined with transition metal (TM = Fe, Co and Ni) catalysts can overcome this difficulty by utilizing functionalities arising from concerted role of active defects on the support surface and loaded transition metals. These catalysts enable ammonia production through multiple reaction pathways. The reaction rate of Co/SrNH is as high as 1686.7 mmol center dot gCo-1 center dot h-1 and the TOFs reaches above 500 h-1 at 400 degrees C and 0.9 MPa, outperforming other reported Co-based catalysts as well as the benchmark Cs-Ru/MgO catalyst and industrial wustite-based Fe catalyst under the same reaction conditions. Experimental and theoretical results show that the synergistic effect of nitrogen affinity of 3d TMs and in-situ formed NH2- vacancy of alkali earth imides regulate the reaction pathways of the ammonia production, resulting in distinct catalytic performance different from 3d TMs. It was thus demonstrated that the appropriate combination of metal and support is essential for controlling the reaction pathway and realizing highly active and low cost catalysts for ammonia synthesis.","The presence of electrically active defects on the surface of the support has been shown to be effective for N2 activation. Here the authors discover that electron-rich polyanionic NH2- defect allows for efficient ammonia synthesis via multiple reaction pathway by incorporating various affordable transition metals."]
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收录类别	SCI
语种	英语
资助项目	This work was supported by the National Natural Science Foundation of China (22275121, 22105122), the Science and Technology Commission of Shanghai Municipality (21PJ1407400), Shanghai Municipal Science and Technology Major Project, Shanghai Science and Te["22275121","22105122"] ; National Natural Science Foundation of China[21PJ1407400] ; Science and Technology Commission of Shanghai Municipality[21DZ2260400] ; Shanghai Municipal Science and Technology Major Project, Shanghai Science and Technology Plan[JDSX2022038] ; Open Foundation Commission of Shaoxing Research Institute of Renewable Energy and Molecular Engineering["2023YSTZX01","02161943"] ; project of Jiangxi Academy of Sciences[JPNP21012] ; Shanghai Tech University["JPMJFR203A","JP22H00272","JP21H00019"] ; Japan Society for the Promotion of Science (JSPS)[02110011044171]
WOS研究方向	Science & Technology - Other Topics
WOS类目	Multidisciplinary Sciences
WOS记录号	WOS:001099083700027
出版者	NATURE PORTFOLIO
引用统计	正在获取...
文献类型	期刊论文
条目标识符	https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/347854
专题	物质科学与技术学院物质科学与技术学院_PI研究组_齐彦鹏组
通讯作者	Kitano, Masaaki; Hosono, Hideo; Ye, Tian-Nan
作者单位	1.Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, Frontiers Sci Ctr Transformat Mol, Shanghai 200240, Peoples R China 2.Chongqing Univ, Coll Mat Sci & Engn, Natl Engn Res Ctr Magnesium Alloys, Chongqing 400044, Peoples R China 3.Tokyo Inst Technol, Mat Res Ctr Element Strategy, 4259 Nagatsuta,Midori Ku, Yokohama 2268503, Japan 4.Shanghai Inst Space Power Sources, State Key Lab Space Power Sources, Shanghai 200245, Peoples R China 5.Shanghai Tech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China 6.ShanghaiTech Univ, ShanghaiTech Lab Topol Phys, Shanghai 201210, Peoples R China 7.ShanghaiTech Univ, Shanghai Key Lab High Resolut Electron Microscopy, Shanghai 201210, Peoples R China
推荐引用方式 GB/T 7714	Li, Zichuang,Lu, Yangfan,Li, Jiang,et al. Multiple reaction pathway on alkaline earth imide supported catalysts for efficient ammonia synthesis[J]. NATURE COMMUNICATIONS,2023,14(1).
APA	Li, Zichuang.,Lu, Yangfan.,Li, Jiang.,Xu, Miao.,Qi, Yanpeng.,...&Ye, Tian-Nan.(2023).Multiple reaction pathway on alkaline earth imide supported catalysts for efficient ammonia synthesis.NATURE COMMUNICATIONS,14(1).
MLA	Li, Zichuang,et al."Multiple reaction pathway on alkaline earth imide supported catalysts for efficient ammonia synthesis".NATURE COMMUNICATIONS 14.1(2023).