Residential College | false |
Status | 已發表Published |
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 Publication | ACS Catalysis |
ISSN | 2155-5435 |
Volume | 13Issue: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. |
Keyword | Ammonia Synthesis Diporphyrins Microkinetic Modeling Milder Conditions Scaling Relations |
DOI | 10.1021/acscatal.3c03160 |
URL | View the original |
Indexed By | SCIE |
Language | 英語English |
WOS Research Area | Chemistry |
WOS Subject | Chemistry, Physical |
WOS ID | WOS:001089470400001 |
Publisher | AMER CHEMICAL SOC1155 16TH ST, NW, WASHINGTON, DC 20036 |
Scopus ID | 2-s2.0-85176151379 |
Fulltext Access | |
Citation statistics | |
Document Type | Journal article |
Collection | DEPARTMENT OF PHYSICS AND CHEMISTRY INSTITUTE OF APPLIED PHYSICS AND MATERIALS ENGINEERING |
Corresponding Author | Kou, Liangzhi; Ng, Kar Wei; Wang, Shuangpeng; Frauenheim, Thomas; Pan, Hui |
Affiliation | 1.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 Affilication | INSTITUTE OF APPLIED PHYSICS AND MATERIALS ENGINEERING |
Corresponding Author Affilication | INSTITUTE 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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