DataVXSmallPaper
journal article·2025-10Open access

Directed Structural Evolution of Nickel Nanoparticles into Atomically Dispersed Sites for Efficient CO 2 Electroreduction.

Xiao Li, Tao Gan, Xinhua Gao, Bing Li, Juan Peng, Yang Ji, Shenghua Chen, Jian Zhang, Junjun Zhang, Pradip Kumar Das, Vinoth Ramalingam, Maolin Zhang, Pengfei Zhang, Karthik Peramaiah, Yajun Qiu

Small· Volume 21· Issue 40
Publisher pageOpen full text
Source abstract

Abstract

Abstract Electrochemical CO 2 reduction (CO 2 RR) to carbon monoxide (CO) offers a sustainable pathway for carbon utilization, yet challenges remain in terms of improving selectivity and activity. Herein, we report a Ni/NC catalyst synthesized via a milling ‐ pyrolysis method, in which Ni particles anchored on nitrogen‐doped carbon (NC) are electrochemically activated under an Ar atmosphere, leading to their structural evolution into single‐atom Ni sites. After activation in Ar atmosphere, the current density nearly doubles (from ≈30 to ≈60 mA cm −2 ), and concurrently, the Faradaic efficiency of CO stays at ∼90% with the potential set to ‐0.8 V vs. RHE. Comprehensive characterizations, including X‐ray photoelectron spectroscopy (XPS), aberration ‐ corrected scanning transmission electron microscopy (AC ‐ STEM), along with extended X ‐ ray absorption fine structure (EXAFS), confirm the change of Ni particles into atomically dispersed Ni‐N x moieties during activation. Notably, in situ Raman spectroscopy identifies * COOH as the key intermediate, while electrochemical analyses reveal accelerated charge transfer and favorable kinetics for Ar‐Ni/NC. Additionally, the catalyst shows great selectivity and stability over 24 hours of non ‐ stop operation. This study emphasizes the dynamic change of Ni active sites under working conditions, offering useful ideas for designing transition metal catalysts for large ‐ scale CO 2 to CO conversion.
Source: crossref · Quality: baseline

Research context

NanomaterialsCatalysis & surfaces

OpenAlex topics: CO2 Reduction Techniques and Catalysts · Ionic liquids properties and applications · Molecular Junctions and Nanostructures

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

State Key Laboratory of High‐efficiency Utilization of Coal and Green Chemical Engineering College of Chemistry and Chemical Engineering Ningxia University Yinchuan Ningxia 750021 P. R. China

Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201204 P. R. China

School of Chemistry National Innovation Platform (Center) for Industry‐Education Integration of Energy Storage Technology Xi'an Jiaotong University Xi'an 710049 P. R. China

Key Laboratory of Carbon Materials of Zhejiang Province Key Lab of Biohealth Materials and Chemistry of Wenzhou College of Chemistry and Materials Engineering Wenzhou University Wenzhou Zhejiang 325035 P. R. China

Institute of Institute of Sustainability for Chemicals Energy, and Environment (ISCE2) Agency for Science, Technology and Research (A*STAR) 1 Pesek Road Singapore 627833 Singapore

School of Computing Engineering and Technology Robert Gordon University Garthdee Road Aberdeen AB10 7GJ UK

Institute of Environment and Sustainable Development in Agriculture Chinese Academy of Agricultural Sciences Beijing 100081 P. R. China

School of Chemistry and Chemical Engineering Shanghai Jiao Tong University Shanghai 200240 P. R. China

References (75)

Show source-provided references
1. 10.1016/j.apcatb.2020.11892910.1016/j.apcatb.2020.118929 ↗
2. 10.1021/jacs.2c0917010.1021/jacs.2c09170 ↗
3. 10.1002/adma.20150476610.1002/adma.201504766 ↗
4. 10.1002/advs.20170027510.1002/advs.201700275 ↗
5. 10.1021/jacs.3c0365110.1021/jacs.3c03651 ↗
6. 10.1038/s41467-017-01035-z10.1038/s41467-017-01035-z ↗
7. Chen Y. · Angew. Chem., Int. Ed. · 2024
8. 10.1016/j.fuel.2022.12404310.1016/j.fuel.2022.124043 ↗
9. Zhou C. · ACS Appl. Mater. Interfaces. · 2023 · 15
10. 10.1021/jacs.4c1132610.1021/jacs.4c11326 ↗
11. 10.1007/s12274-023-5513-510.1007/s12274-023-5513-5 ↗
12. 10.1038/s41565-022-01154-910.1038/s41565-022-01154-9 ↗
13. 10.1016/j.asems.2023.10007310.1016/j.asems.2023.100073 ↗
14. 10.1002/smll.20230112810.1002/smll.202301128 ↗
15. 10.1021/jacs.6b1210310.1021/jacs.6b12103 ↗
16. 10.1002/anie.20191652010.1002/anie.201916520 ↗
17. 10.1002/aenm.20210147710.1002/aenm.202101477 ↗
18. Wen C. F. · Appl. Catal. · 2019 · 10 · 1086
19. 10.1016/j.nanoen.2023.10838410.1016/j.nanoen.2023.108384 ↗
20. 10.1002/anie.20150209910.1002/anie.201502099 ↗
21. 10.1021/acs.energyfuels.4c0116310.1021/acs.energyfuels.4c01163 ↗
22. Cheng Y. · Adv. Mater. · 2018 · 30
23. 10.1002/adma.20180206610.1002/adma.201802066 ↗
24. 10.1021/jacs.1c0805010.1021/jacs.1c08050 ↗
25. 10.1002/adfm.20231682410.1002/adfm.202316824 ↗
26. 10.1002/adfm.20221465810.1002/adfm.202214658 ↗
27. 10.1002/aenm.20220184310.1002/aenm.202201843 ↗
28. 10.1016/j.apcatb.2024.12369910.1016/j.apcatb.2024.123699 ↗
29. 10.1002/anie.20220149110.1002/anie.202201491 ↗
30. 10.1002/anie.20242455210.1002/anie.202424552 ↗
31. 10.1016/j.nanoen.2022.10719110.1016/j.nanoen.2022.107191 ↗
32. 10.1002/adfm.20220235110.1002/adfm.202202351 ↗
33. 10.1039/D4TA02800G10.1039/D4TA02800G ↗
34. Qi L. · J. Am. Chem. Soc. · 2024 · 146
35. Gao Y. · J. Am. Chem. Soc. · 2024 · 146
36. 10.1002/anie.20180804910.1002/anie.201808049 ↗
37. 10.1002/anie.20241826910.1002/anie.202418269 ↗
38. 10.1038/s41467-018-03896-410.1038/s41467-018-03896-4 ↗
39. 10.1016/j.apcatb.2024.12401410.1016/j.apcatb.2024.124014 ↗
40. 10.1016/j.cattod.2015.06.00910.1016/j.cattod.2015.06.009 ↗
41. 10.1002/anie.20250588310.1002/anie.202505883 ↗
42. Ren W. · Angew. Chem., Int. Ed. · 2022
43. 10.1016/j.nanoen.2019.10423310.1016/j.nanoen.2019.104233 ↗
44. 10.1002/anie.20190739910.1002/anie.201907399 ↗
45. 10.1007/s12274-023-5626-x10.1007/s12274-023-5626-x ↗
46. 10.1002/ange.20191497710.1002/ange.201914977 ↗
47. 10.1038/s41560-017-0078-810.1038/s41560-017-0078-8 ↗
48. 10.1016/j.joule.2018.10.01510.1016/j.joule.2018.10.015 ↗
49. 10.1016/j.apcatb.2022.12109310.1016/j.apcatb.2022.121093 ↗
50. 10.1021/jacs.7b0273610.1021/jacs.7b02736 ↗
51. 10.1038/s41467-023-39505-210.1038/s41467-023-39505-2 ↗
52. 10.1039/D0EE03947K10.1039/D0EE03947K ↗
53. 10.1016/j.esci.2023.10013810.1016/j.esci.2023.100138 ↗
54. 10.1016/j.snb.2022.13186710.1016/j.snb.2022.131867 ↗
55. 10.1007/s12598-022-02247-z10.1007/s12598-022-02247-z ↗
56. 10.1021/acsanm.4c0095510.1021/acsanm.4c00955 ↗
57. 10.1021/acssuschemeng.1c0385810.1021/acssuschemeng.1c03858 ↗
58. 10.1021/jacs.7b0841610.1021/jacs.7b08416 ↗
59. 10.1021/acsenergylett.1c0271110.1021/acsenergylett.1c02711 ↗
60. 10.1039/D3TA07216A10.1039/D3TA07216A ↗
61. 10.1016/j.apcatb.2018.10.04610.1016/j.apcatb.2018.10.046 ↗
62. 10.1021/jacs.1c0015110.1021/jacs.1c00151 ↗
63. 10.1016/j.nanoen.2020.10568910.1016/j.nanoen.2020.105689 ↗
64. 10.1002/adma.20170661710.1002/adma.201706617 ↗
65. Fan Q. · Adv. Energy Mater. · 2019 · 10
66. 10.1002/smll.20241072310.1002/smll.202410723 ↗
67. 10.1002/anie.20191199510.1002/anie.201911995 ↗
68. 10.1021/jacs.1c1221210.1021/jacs.1c12212 ↗
69. 10.1002/smll.20230566610.1002/smll.202305666 ↗
70. 10.1007/s12274-022-4623-910.1007/s12274-022-4623-9 ↗
71. 10.1002/adma.20230069510.1002/adma.202300695 ↗
72. 10.1016/j.apcatb.2025.12515110.1016/j.apcatb.2025.125151 ↗
73. 10.1016/j.nanoen.2023.10856810.1016/j.nanoen.2023.108568 ↗
74. Fu X. · Small · 2022 · 18
75. 10.31635/ccschem.023.20230333310.31635/ccschem.023.202303333 ↗