Gram‐Scale Preparation of Tri‐Coordinated Single‐Atom Catalysts for CO2 Electrolysis in Large‐Scale Membrane Electrode Assembly
Abstract Accelerating the commercialization of CO2 electroreduction is essential for carbon utilization, yet it faces challenges of precious metal catalysts cost and scaling‐up of the corresponding devices. In this study, a low‐cost and tri‐coordinated single‐atom catalyst (SAC) with Ni‐N3 center is...
Saved in:
| Main Authors: | , , , , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Wiley
2025-05-01
|
| Series: | Advanced Science |
| Subjects: | |
| Online Access: | https://doi.org/10.1002/advs.202500368 |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1850122735142830080 |
|---|---|
| author | Lei Yuan Xin Li Guilin Li Kuilin Peng Hongyu Zhang Shaojuan Zeng Xiaofu Sun Xiangping Zhang |
| author_facet | Lei Yuan Xin Li Guilin Li Kuilin Peng Hongyu Zhang Shaojuan Zeng Xiaofu Sun Xiangping Zhang |
| author_sort | Lei Yuan |
| collection | DOAJ |
| description | Abstract Accelerating the commercialization of CO2 electroreduction is essential for carbon utilization, yet it faces challenges of precious metal catalysts cost and scaling‐up of the corresponding devices. In this study, a low‐cost and tri‐coordinated single‐atom catalyst (SAC) with Ni‐N3 center is fabricated in gram‐scale using metal ionic liquids as precursor. The gram‐scale Ni‐N3 SAC (g‐NiN3) achieves efficient electroreduction of CO2 to CO (eCO2‐to‐CO) with a maximum Faradaic efficiency of 98.9% at 2.8 V in a 2 × 2 cm2 membrane electrode assembly (MEA) cell, and CO selectivity exceeds 90% during 100 h electrolysis at 100 mA·cm−2. Moreover, the g‐NiN3 is tested in a scale‐up MEA reactor (10 × 10 cm2), which can not only show 97.1% CO Faradaic efficiency with a reaction current of 6.07 A but also achieves a CO2 single‐pass conversion of 41.0%, corresponding to energy efficiency of the system as high as 43.1%. The overall performance of g‐NiN3 is one of the state‐of‐the‐art systems for eCO2‐to‐CO. In addition, the scale‐up device stably generates CO at a high rate of 12.0 L·kW·h−1 over continuous CO2 electrolysis. The techno‐economic assessment demonstrates that the eCO2‐to‐CO using g‐NiN3 can realize CO production cost of 1.08 $·kg−1, and shows great profitability prospects in the future. |
| format | Article |
| id | doaj-art-78f2f287fd3b4f76bb5bb67a5861dfc4 |
| institution | OA Journals |
| issn | 2198-3844 |
| language | English |
| publishDate | 2025-05-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj-art-78f2f287fd3b4f76bb5bb67a5861dfc42025-08-20T02:34:47ZengWileyAdvanced Science2198-38442025-05-011218n/an/a10.1002/advs.202500368Gram‐Scale Preparation of Tri‐Coordinated Single‐Atom Catalysts for CO2 Electrolysis in Large‐Scale Membrane Electrode AssemblyLei Yuan0Xin Li1Guilin Li2Kuilin Peng3Hongyu Zhang4Shaojuan Zeng5Xiaofu Sun6Xiangping Zhang7Beijing Key Laboratory of Ionic Liquids Clean Process State Key Laboratory of Multiphase Complex Systems Key Laboratory of Green Process and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 ChinaBeijing Key Laboratory of Ionic Liquids Clean Process State Key Laboratory of Multiphase Complex Systems Key Laboratory of Green Process and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 ChinaBeijing Key Laboratory of Ionic Liquids Clean Process State Key Laboratory of Multiphase Complex Systems Key Laboratory of Green Process and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 ChinaBeijing Key Laboratory of Ionic Liquids Clean Process State Key Laboratory of Multiphase Complex Systems Key Laboratory of Green Process and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 ChinaBeijing Key Laboratory of Ionic Liquids Clean Process State Key Laboratory of Multiphase Complex Systems Key Laboratory of Green Process and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 ChinaBeijing Key Laboratory of Ionic Liquids Clean Process State Key Laboratory of Multiphase Complex Systems Key Laboratory of Green Process and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 ChinaInstitute of Chemistry Chinese Academy of Sciences Beijing 100190 ChinaBeijing Key Laboratory of Ionic Liquids Clean Process State Key Laboratory of Multiphase Complex Systems Key Laboratory of Green Process and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 ChinaAbstract Accelerating the commercialization of CO2 electroreduction is essential for carbon utilization, yet it faces challenges of precious metal catalysts cost and scaling‐up of the corresponding devices. In this study, a low‐cost and tri‐coordinated single‐atom catalyst (SAC) with Ni‐N3 center is fabricated in gram‐scale using metal ionic liquids as precursor. The gram‐scale Ni‐N3 SAC (g‐NiN3) achieves efficient electroreduction of CO2 to CO (eCO2‐to‐CO) with a maximum Faradaic efficiency of 98.9% at 2.8 V in a 2 × 2 cm2 membrane electrode assembly (MEA) cell, and CO selectivity exceeds 90% during 100 h electrolysis at 100 mA·cm−2. Moreover, the g‐NiN3 is tested in a scale‐up MEA reactor (10 × 10 cm2), which can not only show 97.1% CO Faradaic efficiency with a reaction current of 6.07 A but also achieves a CO2 single‐pass conversion of 41.0%, corresponding to energy efficiency of the system as high as 43.1%. The overall performance of g‐NiN3 is one of the state‐of‐the‐art systems for eCO2‐to‐CO. In addition, the scale‐up device stably generates CO at a high rate of 12.0 L·kW·h−1 over continuous CO2 electrolysis. The techno‐economic assessment demonstrates that the eCO2‐to‐CO using g‐NiN3 can realize CO production cost of 1.08 $·kg−1, and shows great profitability prospects in the future.https://doi.org/10.1002/advs.202500368CO2 electroreductionionic liquidssingle‐atom catalystscale‐uptechno‐economic assessment |
| spellingShingle | Lei Yuan Xin Li Guilin Li Kuilin Peng Hongyu Zhang Shaojuan Zeng Xiaofu Sun Xiangping Zhang Gram‐Scale Preparation of Tri‐Coordinated Single‐Atom Catalysts for CO2 Electrolysis in Large‐Scale Membrane Electrode Assembly Advanced Science CO2 electroreduction ionic liquids single‐atom catalyst scale‐up techno‐economic assessment |
| title | Gram‐Scale Preparation of Tri‐Coordinated Single‐Atom Catalysts for CO2 Electrolysis in Large‐Scale Membrane Electrode Assembly |
| title_full | Gram‐Scale Preparation of Tri‐Coordinated Single‐Atom Catalysts for CO2 Electrolysis in Large‐Scale Membrane Electrode Assembly |
| title_fullStr | Gram‐Scale Preparation of Tri‐Coordinated Single‐Atom Catalysts for CO2 Electrolysis in Large‐Scale Membrane Electrode Assembly |
| title_full_unstemmed | Gram‐Scale Preparation of Tri‐Coordinated Single‐Atom Catalysts for CO2 Electrolysis in Large‐Scale Membrane Electrode Assembly |
| title_short | Gram‐Scale Preparation of Tri‐Coordinated Single‐Atom Catalysts for CO2 Electrolysis in Large‐Scale Membrane Electrode Assembly |
| title_sort | gram scale preparation of tri coordinated single atom catalysts for co2 electrolysis in large scale membrane electrode assembly |
| topic | CO2 electroreduction ionic liquids single‐atom catalyst scale‐up techno‐economic assessment |
| url | https://doi.org/10.1002/advs.202500368 |
| work_keys_str_mv | AT leiyuan gramscalepreparationoftricoordinatedsingleatomcatalystsforco2electrolysisinlargescalemembraneelectrodeassembly AT xinli gramscalepreparationoftricoordinatedsingleatomcatalystsforco2electrolysisinlargescalemembraneelectrodeassembly AT guilinli gramscalepreparationoftricoordinatedsingleatomcatalystsforco2electrolysisinlargescalemembraneelectrodeassembly AT kuilinpeng gramscalepreparationoftricoordinatedsingleatomcatalystsforco2electrolysisinlargescalemembraneelectrodeassembly AT hongyuzhang gramscalepreparationoftricoordinatedsingleatomcatalystsforco2electrolysisinlargescalemembraneelectrodeassembly AT shaojuanzeng gramscalepreparationoftricoordinatedsingleatomcatalystsforco2electrolysisinlargescalemembraneelectrodeassembly AT xiaofusun gramscalepreparationoftricoordinatedsingleatomcatalystsforco2electrolysisinlargescalemembraneelectrodeassembly AT xiangpingzhang gramscalepreparationoftricoordinatedsingleatomcatalystsforco2electrolysisinlargescalemembraneelectrodeassembly |