Citation: Ya Ren, Cong Zhang, Haiyan Wang, Jin-Xia Liang, Chun Zhu, Han-Shi Hu, Jun Li. Defective Ru1@Mo2COx Single-Atom Catalyst for Efﬁcient Thermal Catalysis for Ammonia Synthesis[J]. Chinese Journal of Structural Chemistry, ;2025, 44(8): 100649. doi: 10.1016/j.cjsc.2025.100649 shu

Defective Ru1@Mo2COx Single-Atom Catalyst for Efﬁcient Thermal Catalysis for Ammonia Synthesis

The reduction of N2 to NH3 is an important reaction for the industrial production of ammonia gas. Here, we theoretically studied the thermal synthesis of ammonia catalyzed by Ru1@Mo2COx single-atom catalyst, where Ru atoms are anchored on the oxygen vacancy of the defective Mo2COx. The results show that Ru1@Mo2COx exhibits excellent stability. Moreover, Ru1@Mo2COx can effectively adsorb and activate N2, owing to up to −0.87 |e| charge transfer from Ru1@Mo2COx to N2. The optimal pathway of N2-to-NH3 conversion is association pathway I, of which the rate-determining step is *NH2→*NH3 with of barrier energy of 1.26 eV. Especially, the Mo2COx center functions as an electron reservoir, donating electrons to the NxHy species, while the Ru single atom serves as a charge transfer pathway, thereby enhancing the reaction activity. This finding provides a theoretical foundation for the rational design of MXene-based single-atom catalysts for thermal catalytic NH3 synthesis.
- N2-to-NH3 conversion,
- Single-atom catalyst,
- DFT,
- MXene,
- Ru1@Mo2COx
1. [1]
  Xiangyuan Zhao , Jinjin Wang , Jinzhao Kang , Xiaomei Wang , Hong Yu , Cheng-Feng Du . Ni nanoparticles anchoring on vacuum treated Mo2TiC2Tx MXene for enhanced hydrogen evolution activity. Chinese Journal of Structural Chemistry, 2023, 42(10): 100159-100159. doi: 10.1016/j.cjsc.2023.100159
2. [2]
  Fan Yang , Zheng Liu , Da Wang , KwunNam Hui , Yelong Zhang , Zhangquan Peng . Preparation and Properties of P-Bi₂Te₃/MXene Superstructure-based Anode for Potassium-Ion Battery. Acta Physico-Chimica Sinica, 2024, 40(2): 2303006-0. doi: 10.3866/PKU.WHXB202303006
3. [3]
  Qian-Qian Tang , Li-Fang Feng , Zhi-Peng Li , Shi-Hao Wu , Long-Shuai Zhang , Qing Sun , Mei-Feng Wu , Jian-Ping Zou . Single-atom sites regulation by the second-shell doping for efficient electrochemical CO₂ reduction. Chinese Chemical Letters, 2024, 35(9): 109454-. doi: 10.1016/j.cclet.2023.109454
4. [4]
  Tsegaye Tadesse Tsega , Jiantao Zai , Chin Wei Lai , Xin-Hao Li , Xuefeng Qian . Earth-abundant CuFeS2 nanocrystals@graphite felt electrode for high performance aqueous polysulfide/iodide redox flow batteries. Chinese Journal of Structural Chemistry, 2024, 43(1): 100192-100192. doi: 10.1016/j.cjsc.2023.100192
5. [5]
  Kun Rong , Cuilian Wen , Jiansen Wen , Xiong Li , Qiugang Liao , Siqing Yan , Chao Xu , Xiaoliang Zhang , Baisheng Sa , Zhimei Sun . Hierarchical MoS₂/Ti₃C₂T_x heterostructure with excellent photothermal conversion performance for solar-driven vapor generation. Acta Physico-Chimica Sinica, 2025, 41(6): 100053-0. doi: 10.1016/j.actphy.2025.100053
6. [6]
  Minying Wu , Xueliang Fan , Wenbiao Zhang , Bin Chen , Tong Ye , Qian Zhang , Yuanyuan Fang , Yajun Wang , Yi Tang . Highly dispersed Ru nanospecies on N-doped carbon/MXene composite for highly efficient alkaline hydrogen evolution. Chinese Chemical Letters, 2024, 35(4): 109258-. doi: 10.1016/j.cclet.2023.109258
7. [7]
  Tong Su , Yue Wang , Qizhen Zhu , Mengyao Xu , Ning Qiao , Bin Xu . Multiple conductive network for KTi₂(PO₄)₃ anode based on MXene as a binder for high-performance potassium storage. Chinese Chemical Letters, 2024, 35(8): 109191-. doi: 10.1016/j.cclet.2023.109191
8. [8]
  Haiyan Wang , Hucheng Zhang , Lijing Wang , Yonghui Li , Tianhao Zhang , Zhansheng Lu , Hao Jiang , Chunzhong Li , Jianji Wang . Ti₃C₂T_x MXene-mediating near- and long-range electronic effect on atomically dispersed Co for efficient lithium-sulfur batteries. Chinese Chemical Letters, 2025, 36(10): 110373-. doi: 10.1016/j.cclet.2024.110373
9. [9]
  Yaping Wang , Pengcheng Yuan , Zeyuan Xu , Xiong-Xiong Liu , Shengfa Feng , Mufan Cao , Chen Cao , Xiaoqiang Wang , Long Pan , Zheng-Ming Sun . Ti₃C₂T_x MXene in-situ transformed Li₂TiO₃ interface layer enabling 4.5 V-LiCoO₂/sulfide all-solid-state lithium batteries with superior rate capability and cyclability. Chinese Chemical Letters, 2024, 35(6): 108776-. doi: 10.1016/j.cclet.2023.108776
10. [10]
  Fangling Cui , Zongjie Hu , Jiayu Huang , Xiaoju Li , Ruihu Wang . MXene-based materials for separator modification of lithium-sulfur batteries. Chinese Journal of Structural Chemistry, 2024, 43(7): 100337-100337. doi: 10.1016/j.cjsc.2024.100337
11. [11]
  Chunyan Yang , Qiuyu Rong , Fengyin Shi , Menghan Cao , Guie Li , Yanjun Xin , Wen Zhang , Guangshan Zhang . Rationally designed S-scheme heterojunction of BiOCl/g-C₃N₄ for photodegradation of sulfamerazine: Mechanism insights, degradation pathways and DFT calculation. Chinese Chemical Letters, 2024, 35(12): 109767-. doi: 10.1016/j.cclet.2024.109767
12. [12]
  Changle Liu , Mingyuzhi Sun , Haoran Zhang , Xiqian Cao , Yuqing Li , Yingtang Zhou . All in one doubly pillared MXene membrane for excellent oil/water separation, pollutant removal, and anti-fouling performance. Chinese Journal of Structural Chemistry, 2024, 43(8): 100355-100355. doi: 10.1016/j.cjsc.2024.100355
13. [13]
  Sanmei Wang , Yong Zhou , Hengxin Fang , Chunyang Nie , Chang Q Sun , Biao Wang . Constant-potential simulation of electrocatalytic N₂ reduction over atomic metal-N-graphene catalysts. Chinese Chemical Letters, 2025, 36(3): 110476-. doi: 10.1016/j.cclet.2024.110476
14. [14]
  Chaozheng He , Jia Wang , Ling Fu , Wei Wei . Nitric oxide assists nitrogen reduction reaction on 2D MBene: A theoretical study. Chinese Chemical Letters, 2024, 35(5): 109037-. doi: 10.1016/j.cclet.2023.109037
15. [15]
  Ting-Ting Huang , Jin-Fa Chen , Juan Liu , Tai-Bao Wei , Hong Yao , Bingbing Shi , Qi Lin . A novel fused bi-macrocyclic host for sensitive detection of Cr₂O₇²⁻ based on enrichment effect. Chinese Chemical Letters, 2024, 35(7): 109281-. doi: 10.1016/j.cclet.2023.109281
16. [16]
  Sanmei Wang , Dengxin Yan , Wenhua Zhang , Liangbing Wang . Graphene-supported isolated platinum atoms and platinum dimers for CO₂ hydrogenation: Catalytic activity and selectivity variations. Chinese Chemical Letters, 2025, 36(4): 110611-. doi: 10.1016/j.cclet.2024.110611
17. [17]
  Lina Zou , Dengke Wang , Shiqin Lai , Xunheng Jiang , Siqi Chen , Lanqing Deng , Dong Fan , Hengshuai Li , Zhigang Zhou , Denglong Chen , Xiangyang Yao , Jianping Zou . Local spin-state manipulation of iron single-atom sites induced by sulfur modification to boost Fenton-like reaction. Chinese Chemical Letters, 2025, 36(12): 111094-. doi: 10.1016/j.cclet.2025.111094
18. [18]
  Zhengyu Zhou , Huiqin Yao , Youlin Wu , Teng Li , Noritatsu Tsubaki , Zhiliang Jin . Synergistic Effect of Cu-Graphdiyne/Transition Bimetallic Tungstate Formed S-Scheme Heterojunction for Enhanced Photocatalytic Hydrogen Evolution. Acta Physico-Chimica Sinica, 2024, 40(10): 2312010-0. doi: 10.3866/PKU.WHXB202312010
19. [19]
  Rohit Kumar , Anita Sudhaik , Aftab Asalam Pawaz Khan , Van Huy Neguyen , Archana Singh , Pardeep Singh , Sourbh Thakur , Pankaj Raizada . Designing tandem S-scheme photo-catalytic systems: Mechanistic insights, characterization techniques, and applications. Acta Physico-Chimica Sinica, 2025, 41(11): 100150-0. doi: 10.1016/j.actphy.2025.100150
20. [20]
  Shasha SUN , Weichun HUANG , Mengke WANG . Research progress of interface regulation strategies and applications of two‑dimensional MXenes. Chinese Journal of Inorganic Chemistry, 2025, 41(8): 1465-1482. doi: 10.11862/CJIC.20240430

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(2)
HTML views(1)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Address：Zhongguancun North First Street 2,100190 Beijing, PR China Tel: +86-010-82449177-888

DownLoad: Full-Size Img PowerPoint

Return