Isolated FeN3 sites anchored hierarchical porous carbon nanoboxes for hydrazine‐assisted rechargeable Zn‐CO2 batteries with ultralow charge voltage
Abstract Zn‐CO2 batteries (ZCBs) are promising for CO2 conversion and electric energy release. However, the ZCBs couple the electrochemical CO2 reduction (ECO2R) with the oxygen evolution reaction and competitive hydrogen evolution reaction, which normally causes ultrahigh charge voltage and CO2 con...
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| Format: | Article |
| Language: | English |
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Wiley
2025-01-01
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| Series: | Carbon Energy |
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| Online Access: | https://doi.org/10.1002/cey2.637 |
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| author | Sanshuang Gao Hongyi Li Zhansheng Lu Songjie Meng Xue Zhao Xinzhong Wang Xijun Liu Guangzhi Hu |
| author_facet | Sanshuang Gao Hongyi Li Zhansheng Lu Songjie Meng Xue Zhao Xinzhong Wang Xijun Liu Guangzhi Hu |
| author_sort | Sanshuang Gao |
| collection | DOAJ |
| description | Abstract Zn‐CO2 batteries (ZCBs) are promising for CO2 conversion and electric energy release. However, the ZCBs couple the electrochemical CO2 reduction (ECO2R) with the oxygen evolution reaction and competitive hydrogen evolution reaction, which normally causes ultrahigh charge voltage and CO2 conversion efficiency attenuation, thereby resulting in ~90% total power consumption. Herein, isolated FeN3 sites encapsulated in hierarchical porous carbon nanoboxes (Fe‐HPCN, derived from the thermal activation process of ferrocene and polydopamine‐coated cubic ZIF‐8) were proposed for hydrazine‐assisted rechargeable ZCBs based on ECO2R (discharging process: CO2 + 2H+ → CO + H2O) and hydrazine oxidation reaction (HzOR, charging process: N2H4 + 4OH− → N2 + 4H2O + 4e−). The isolated FeN3 endows the HzOR with a lower overpotential and boosts the ECO2R with a 96% CO Faraday efficiency (FECO). Benefitting from the bifunctional ECO2R and HzOR catalytic activities, the homemade hydrazine‐assisted rechargeable ZCBs assembled with the Fe‐HPCN air cathode exhibited an ultralow charge voltage (decreasing by ~1.84 V), excellent CO selectivity (FECO close to 100%), and high 89% energy efficiency. In situ infrared spectroscopy confirmed that Fe‐HPCN can generate rate‐determining *N2 and *CO intermediates during HzOR and ECO2R. This paper proposes FeN3 centers for bifunctional ECO2R/HzOR performance and further presents the pioneering achievements of ECO2R and HzOR for hydrazine‐assisted rechargeable ZCBs. |
| format | Article |
| id | doaj-art-8d81a3882eb847e2abb11e7f9f7d1e66 |
| institution | Kabale University |
| issn | 2637-9368 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Wiley |
| record_format | Article |
| series | Carbon Energy |
| spelling | doaj-art-8d81a3882eb847e2abb11e7f9f7d1e662025-01-24T13:35:41ZengWileyCarbon Energy2637-93682025-01-0171n/an/a10.1002/cey2.637Isolated FeN3 sites anchored hierarchical porous carbon nanoboxes for hydrazine‐assisted rechargeable Zn‐CO2 batteries with ultralow charge voltageSanshuang Gao0Hongyi Li1Zhansheng Lu2Songjie Meng3Xue Zhao4Xinzhong Wang5Xijun Liu6Guangzhi Hu7Shenzhen Institute of Information Technology Shenzhen ChinaState Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources, College of Chemistry Xinjiang University Urumqi ChinaSchool of Physics Henan Normal University Xinxiang ChinaSchool of Physics Henan Normal University Xinxiang ChinaFaculty of Chemistry and Chemical Engineering Yunnan Normal University Kunming ChinaShenzhen Institute of Information Technology Shenzhen ChinaState Key Laboratory of Featured Metal Materials and Life‐cycle Safety for Composite Structures, Guangxi Key Laboratory of Processing for Non‐ferrous Metals and Featured Materials, School of Resources, Environment and Materials Guangxi University Nanning ChinaSchool of Ecology and Environmental Science, Institute for Ecological Research and Pollution Control of Plateau Lakes Yunnan University Kunming ChinaAbstract Zn‐CO2 batteries (ZCBs) are promising for CO2 conversion and electric energy release. However, the ZCBs couple the electrochemical CO2 reduction (ECO2R) with the oxygen evolution reaction and competitive hydrogen evolution reaction, which normally causes ultrahigh charge voltage and CO2 conversion efficiency attenuation, thereby resulting in ~90% total power consumption. Herein, isolated FeN3 sites encapsulated in hierarchical porous carbon nanoboxes (Fe‐HPCN, derived from the thermal activation process of ferrocene and polydopamine‐coated cubic ZIF‐8) were proposed for hydrazine‐assisted rechargeable ZCBs based on ECO2R (discharging process: CO2 + 2H+ → CO + H2O) and hydrazine oxidation reaction (HzOR, charging process: N2H4 + 4OH− → N2 + 4H2O + 4e−). The isolated FeN3 endows the HzOR with a lower overpotential and boosts the ECO2R with a 96% CO Faraday efficiency (FECO). Benefitting from the bifunctional ECO2R and HzOR catalytic activities, the homemade hydrazine‐assisted rechargeable ZCBs assembled with the Fe‐HPCN air cathode exhibited an ultralow charge voltage (decreasing by ~1.84 V), excellent CO selectivity (FECO close to 100%), and high 89% energy efficiency. In situ infrared spectroscopy confirmed that Fe‐HPCN can generate rate‐determining *N2 and *CO intermediates during HzOR and ECO2R. This paper proposes FeN3 centers for bifunctional ECO2R/HzOR performance and further presents the pioneering achievements of ECO2R and HzOR for hydrazine‐assisted rechargeable ZCBs.https://doi.org/10.1002/cey2.637electrochemical CO2 reductionFe single atomshierarchical porous carbon nanoboxeshydrazine‐assisted Zn‐CO2 batterieshydrazine oxidation reaction |
| spellingShingle | Sanshuang Gao Hongyi Li Zhansheng Lu Songjie Meng Xue Zhao Xinzhong Wang Xijun Liu Guangzhi Hu Isolated FeN3 sites anchored hierarchical porous carbon nanoboxes for hydrazine‐assisted rechargeable Zn‐CO2 batteries with ultralow charge voltage Carbon Energy electrochemical CO2 reduction Fe single atoms hierarchical porous carbon nanoboxes hydrazine‐assisted Zn‐CO2 batteries hydrazine oxidation reaction |
| title | Isolated FeN3 sites anchored hierarchical porous carbon nanoboxes for hydrazine‐assisted rechargeable Zn‐CO2 batteries with ultralow charge voltage |
| title_full | Isolated FeN3 sites anchored hierarchical porous carbon nanoboxes for hydrazine‐assisted rechargeable Zn‐CO2 batteries with ultralow charge voltage |
| title_fullStr | Isolated FeN3 sites anchored hierarchical porous carbon nanoboxes for hydrazine‐assisted rechargeable Zn‐CO2 batteries with ultralow charge voltage |
| title_full_unstemmed | Isolated FeN3 sites anchored hierarchical porous carbon nanoboxes for hydrazine‐assisted rechargeable Zn‐CO2 batteries with ultralow charge voltage |
| title_short | Isolated FeN3 sites anchored hierarchical porous carbon nanoboxes for hydrazine‐assisted rechargeable Zn‐CO2 batteries with ultralow charge voltage |
| title_sort | isolated fen3 sites anchored hierarchical porous carbon nanoboxes for hydrazine assisted rechargeable zn co2 batteries with ultralow charge voltage |
| topic | electrochemical CO2 reduction Fe single atoms hierarchical porous carbon nanoboxes hydrazine‐assisted Zn‐CO2 batteries hydrazine oxidation reaction |
| url | https://doi.org/10.1002/cey2.637 |
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