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Three-Dimensional Dual-Site Catalysts for Industrial Ammonia Synthesis at Dramatically Decreased Temperatures and Pressures
Lv, Xingshuai1; Liu, Junxian2; Kou, Liangzhi2; Ng, Kar Wei1; Wang, Shuangpeng1; Frauenheim, Thomas3,4; Pan, Hui1,5
2023-10-06
Source PublicationACS Catalysis
ISSN2155-5435
Volume13Issue:20Pages:13561-13568
Abstract

Industrial ammonia (NH) production via the Haber-Bosch (H-B) process is a great achievement of the 20th century, but its energy-intensive character renders NH production costly. Despite considerable efforts, progress in developing an efficient H-B catalyst that operates under near-ambient conditions has been slow. In this study, we leverage the confinement concept to facilitate low-temperature and low-pressure NH synthesis by constructing three-dimensional (3D) dual-site environments. Through first-principles calculations and microkinetic modeling, we demonstrate that the 3D confined dual site on diporphyrins can surpass the limitations imposed by energy-scaling relations, resulting in a significantly increased turnover frequency (TOF) for NH production. Notably, the calculated TOF is 2-3 orders of magnitude higher than that of the commercial ruthenium catalyst at the same working conditions, thus enabling a much-milder H-B process, e.g., at a dramatically decreased working pressure of 10 bar at 590 K. We believe that the strategy will pave the way for the development of economically viable alternatives to current industrial processes.

KeywordAmmonia Synthesis Diporphyrins Microkinetic Modeling Milder Conditions Scaling Relations
DOI10.1021/acscatal.3c03160
URLView the original
Indexed BySCIE
Language英語English
WOS Research AreaChemistry
WOS SubjectChemistry, Physical
WOS IDWOS:001089470400001
PublisherAMER CHEMICAL SOC1155 16TH ST, NW, WASHINGTON, DC 20036
Scopus ID2-s2.0-85176151379
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Citation statistics
Document TypeJournal article
CollectionDEPARTMENT OF PHYSICS AND CHEMISTRY
INSTITUTE OF APPLIED PHYSICS AND MATERIALS ENGINEERING
Corresponding AuthorKou, Liangzhi; Ng, Kar Wei; Wang, Shuangpeng; Frauenheim, Thomas; Pan, Hui
Affiliation1.Institute of Applied Physics and Materials Engineering, University of Macau, 999078, Macao
2.School of Mechanical, Medical and Process Engineering, Queensland University of Technology, Brisbane, 4001, Australia
3.School of Science, Constructor University, Bremen, 28759, Germany
4.Beijing Computational Science Research Center, Beijing, 100193, China
5.Department of Physics and Chemistry, Faculty of Science and Technology, University of Macau, Macao, 999078, Macao
First Author AffilicationINSTITUTE OF APPLIED PHYSICS AND MATERIALS ENGINEERING
Corresponding Author AffilicationINSTITUTE OF APPLIED PHYSICS AND MATERIALS ENGINEERING;  Faculty of Science and Technology
Recommended Citation
GB/T 7714
Lv, Xingshuai,Liu, Junxian,Kou, Liangzhi,et al. Three-Dimensional Dual-Site Catalysts for Industrial Ammonia Synthesis at Dramatically Decreased Temperatures and Pressures[J]. ACS Catalysis, 2023, 13(20), 13561-13568.
APA Lv, Xingshuai., Liu, Junxian., Kou, Liangzhi., Ng, Kar Wei., Wang, Shuangpeng., Frauenheim, Thomas., & Pan, Hui (2023). Three-Dimensional Dual-Site Catalysts for Industrial Ammonia Synthesis at Dramatically Decreased Temperatures and Pressures. ACS Catalysis, 13(20), 13561-13568.
MLA Lv, Xingshuai,et al."Three-Dimensional Dual-Site Catalysts for Industrial Ammonia Synthesis at Dramatically Decreased Temperatures and Pressures".ACS Catalysis 13.20(2023):13561-13568.
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