Balancing sub‐reaction activity to boost electrocatalytic urea synthesis using a metal‐free electrocatalyst
Source abstract
Abstract
Abstract Electrocatalytic urea synthesis via coupling of nitrate with CO2 is considered as a promising alternative to the industrial urea synthetic process. However, the requirement of sub‐reaction (NO3RR and CO2RR) activities for efficient urea synthesis is not clear and the related reaction mechanisms remain obscure. Here, the construction, breaking, and rebuilding of the sub‐reaction activity balance would be accompanied by the corresponding regulation in urea synthesis, and the balance of sub‐reaction activities was proven to play a vital role in efficient urea synthesis. With rational design, a urea yield rate of 610.6 mg h−1 gcat.−1 was realized on the N‐doped carbon electrocatalyst, superior to that of noble‐metal electrocatalysts. Based on the operando SR‐FTIR measurements, we proposed that urea synthesis arises from the coupling of *NO and *CO to generate the key intermediate of *OCNO. This work provides new insights and guidelines into urea synthesis from the aspect of activity balance.
Source: crossref · Quality: baseline
Research context
OpenAlex topics: Ammonia Synthesis and Nitrogen Reduction · Caching and Content Delivery · Advanced Photocatalysis Techniques
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
State Key Laboratory of Chem/Bio‐Sensing and Chemometrics, Advanced Catalytic Engineering Research Center of the Ministry of Education, College of Chemistry and Chemical Engineering Hunan University Changsha China
College of Chemistry and Materials Science Nanjing Normal University Nanjing China
National Synchrotron Radiation Laboratory University of Science and Technology of China Hefei China
Key Laboratory of Magnetic Resonance in Biological Systems, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan Collaborative Innovation Center of Chemistry for Life Sciences, Wuhan Institute of Physics and Mathematics Chinese Academy of Sciences Wuhan China
Funding
National Natural Science Foundation of China · China Postdoctoral Science Foundation
References (60)
Show source-provided references
1. 10.1126/science.345.6197.61010.1126/science.345.6197.610 ↗
2. 10.1038/s41929-019-0280-010.1038/s41929-019-0280-0 ↗
3. 10.1126/science.aar661110.1126/science.aar6611 ↗
4. 10.1016/j.egypro.2011.02.10710.1016/j.egypro.2011.02.107 ↗
5. 10.1038/s41557-020-0481-910.1038/s41557-020-0481-9 ↗
6. 10.1038/s41893-021-00741-310.1038/s41893-021-00741-3 ↗
7. 10.1002/anie.20210990510.1002/anie.202109905 ↗
8. 10.1002/smll.20180502910.1002/smll.201805029 ↗
9. 10.1021/jacs.7b0889110.1021/jacs.7b08891 ↗
10. 10.1038/s41586-019-1260-x10.1038/s41586-019-1260-x ↗
11. 10.1021/jacs.8b0837910.1021/jacs.8b08379 ↗
12. 10.1038/s41560-020-0654-110.1038/s41560-020-0654-1 ↗
13. 10.1021/jacs.7b0439310.1021/jacs.7b04393 ↗
14. 10.1021/jacs.0c0041810.1021/jacs.0c00418 ↗
15. 10.1021/jacs.8b1316510.1021/jacs.8b13165 ↗
16. 10.1002/anie.20191599210.1002/anie.201915992 ↗
17. 10.1021/acscatal.9b0526010.1021/acscatal.9b05260 ↗
18. 10.1002/anie.20200233710.1002/anie.202002337 ↗
19. 10.1021/acsenergylett.0c0208210.1021/acsenergylett.0c02082 ↗
20. 10.1021/jacs.9b1334710.1021/jacs.9b13347 ↗
21. 10.1007/978-3-319-73645-7_2010.1007/978-3-319-73645-7_20 ↗
22. 10.1016/j.watres.2020.11559610.1016/j.watres.2020.115596 ↗
23. 10.1016/j.watres.2020.11553910.1016/j.watres.2020.115539 ↗
24. 10.1016/j.joule.2020.12.02510.1016/j.joule.2020.12.025 ↗
25. 10.1021/acsenergylett.0c0092410.1021/acsenergylett.0c00924 ↗
26. 10.1021/acssuschemeng.9b0598310.1021/acssuschemeng.9b05983 ↗
27. 10.1021/acs.jpclett.1c0169110.1021/acs.jpclett.1c01691 ↗
28. 10.1002/smsc.20210007010.1002/smsc.202100070 ↗
29. 10.1016/j.ijhydene.2013.09.05410.1016/j.ijhydene.2013.09.054 ↗
30. 10.1002/cssc.20170144810.1002/cssc.201701448 ↗
31. 10.1016/j.xcrp.2021.10037810.1016/j.xcrp.2021.100378 ↗
32. 10.1021/acs.nanolett.0c0340010.1021/acs.nanolett.0c03400 ↗
33. 10.1038/nature1645510.1038/nature16455 ↗
34. 10.1021/jacs.0c0540810.1021/jacs.0c05408 ↗
35. 10.1021/jacs.9b0576610.1021/jacs.9b05766 ↗
36. 10.1016/j.xcrp.2020.10014510.1016/j.xcrp.2020.100145 ↗
37. 10.1016/j.mtphys.2021.10043110.1016/j.mtphys.2021.100431 ↗
38. 10.1021/jacs.9b1112310.1021/jacs.9b11123 ↗
39. 10.1016/j.cej.2021.13141410.1016/j.cej.2021.131414 ↗
40. 10.1002/anie.20181112610.1002/anie.201811126 ↗
41. 10.1038/s41586-019-1871-210.1038/s41586-019-1871-2 ↗
42. 10.1021/jacs.0c0696010.1021/jacs.0c06960 ↗
43. 10.1021/jacs.7b0907410.1021/jacs.7b09074 ↗
44. 10.1103/PhysRevB.59.R658510.1103/PhysRevB.59.R6585 ↗
45. 10.3390/nano1109241810.3390/nano11092418 ↗
46. 10.1016/j.snb.2019.01.03210.1016/j.snb.2019.01.032 ↗
47. 10.1039/C2AN15780B10.1039/C2AN15780B ↗
48. 10.1002/anie.20210127510.1002/anie.202101275 ↗
49. 10.1021/jacs.7b1242010.1021/jacs.7b12420 ↗
50. 10.1016/j.apsusc.2018.12.04310.1016/j.apsusc.2018.12.043 ↗
51. 10.1038/nchem.109510.1038/nchem.1095 ↗
52. 10.1002/adma.20180349810.1002/adma.201803498 ↗
53. 10.1016/j.cej.2021.12895810.1016/j.cej.2021.128958 ↗
54. 10.1021/ie50286a00810.1021/ie50286a008 ↗
55. 10.1039/c0gc00674b10.1039/c0gc00674b ↗
56. 10.1021/la015739g10.1021/la015739g ↗
57. 10.1039/b511978b10.1039/b511978b ↗
58. 10.1063/1.325105510.1063/1.3251055 ↗
59. Interaction of CO and NO with the spinel CuCr2O4 (100) surface: a DFT study
60. 10.1016/j.jcat.2004.08.03910.1016/j.jcat.2004.08.039 ↗