Boosting Nitrogen Reduction Reaction via Electronic Coupling of Atomically Dispersed Bismuth with Titanium Nitride Nanorods
Abstract Electrocatalytic nitrogen reduction reaction (NRR) is a promising alternative to the traditional Haber–Bosch process. However, the sluggish kinetics and competitive hydrogen evolution reaction result in poor NH3 yield and low Faradaic efficiency (FE). Herein, single bismuth atoms incorporat...
| Main Authors: | , , , , , , |
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| Format: | Article |
| Language: | English |
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Wiley
2022-02-01
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| Series: | Advanced Science |
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| Online Access: | https://doi.org/10.1002/advs.202104245 |
| _version_ | 1798030194173280256 |
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| author | Zichao Xi Ke Shi Xuan Xu Peng Jing Baocang Liu Rui Gao Jun Zhang |
| author_facet | Zichao Xi Ke Shi Xuan Xu Peng Jing Baocang Liu Rui Gao Jun Zhang |
| author_sort | Zichao Xi |
| collection | DOAJ |
| description | Abstract Electrocatalytic nitrogen reduction reaction (NRR) is a promising alternative to the traditional Haber–Bosch process. However, the sluggish kinetics and competitive hydrogen evolution reaction result in poor NH3 yield and low Faradaic efficiency (FE). Herein, single bismuth atoms incorporated hollow titanium nitride nanorods encapsulated in nitrogen‐doped carbon layer (NC) supported on carbon cloth (NC/Bi SAs/TiN/CC) is constructed for electrocatalytic NRR. Impressively, as an integrated electrode, it exhibits a superior ammonia yield rate of 76.15 µg mgcat−1 h−1 (9859 µg μmolBi−1 h−1) at −0.8 V versus RHE and a high FE of 24.60% at −0.5 V versus RHE in 0.1 m Na2SO4 solution, which can retain stable performance in 10 h continuous operation, surpassing the overwhelming majority of reported Bi‐based NRR catalysts. Coupling various characterizations with theory calculations, it is disclosed that the unique monolithic core‐shell configuration with porous structure endows abundant accessible active sites, outstanding charge‐transfer property, and good stability, while the cooperation effect of Bi SAs and TiN can simultaneously promote the hydrogenation of N2 into NH3* on the TiN surface and the desorption of NH3* to release NH3 on the Bi SA sites. These features result in the significant promotion of NRR performance. |
| first_indexed | 2024-04-11T19:36:15Z |
| format | Article |
| id | doaj.art-6e027cd3d11747eea115257d3f52e93f |
| institution | Directory Open Access Journal |
| issn | 2198-3844 |
| language | English |
| last_indexed | 2024-04-11T19:36:15Z |
| publishDate | 2022-02-01 |
| publisher | Wiley |
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| series | Advanced Science |
| spelling | doaj.art-6e027cd3d11747eea115257d3f52e93f2022-12-22T04:06:50ZengWileyAdvanced Science2198-38442022-02-0194n/an/a10.1002/advs.202104245Boosting Nitrogen Reduction Reaction via Electronic Coupling of Atomically Dispersed Bismuth with Titanium Nitride NanorodsZichao Xi0Ke Shi1Xuan Xu2Peng Jing3Baocang Liu4Rui Gao5Jun Zhang6School of Chemistry and Chemical Engineering Inner Mongolia Engineering and Technology Research Center for Catalytic Conversion and Utilization of Carbon Resource Molecules and Inner Mongolia Key Lab of Nanoscience and Nanotechnology Inner Mongolia University 235 West University Street Hohhot 010021 P. R. ChinaSchool of Chemistry and Chemical Engineering Inner Mongolia Engineering and Technology Research Center for Catalytic Conversion and Utilization of Carbon Resource Molecules and Inner Mongolia Key Lab of Nanoscience and Nanotechnology Inner Mongolia University 235 West University Street Hohhot 010021 P. R. ChinaSchool of Chemistry and Chemical Engineering Inner Mongolia Engineering and Technology Research Center for Catalytic Conversion and Utilization of Carbon Resource Molecules and Inner Mongolia Key Lab of Nanoscience and Nanotechnology Inner Mongolia University 235 West University Street Hohhot 010021 P. R. ChinaSchool of Chemistry and Chemical Engineering Inner Mongolia Engineering and Technology Research Center for Catalytic Conversion and Utilization of Carbon Resource Molecules and Inner Mongolia Key Lab of Nanoscience and Nanotechnology Inner Mongolia University 235 West University Street Hohhot 010021 P. R. ChinaSchool of Chemistry and Chemical Engineering Inner Mongolia Engineering and Technology Research Center for Catalytic Conversion and Utilization of Carbon Resource Molecules and Inner Mongolia Key Lab of Nanoscience and Nanotechnology Inner Mongolia University 235 West University Street Hohhot 010021 P. R. ChinaSchool of Chemistry and Chemical Engineering Inner Mongolia Engineering and Technology Research Center for Catalytic Conversion and Utilization of Carbon Resource Molecules and Inner Mongolia Key Lab of Nanoscience and Nanotechnology Inner Mongolia University 235 West University Street Hohhot 010021 P. R. ChinaSchool of Chemistry and Chemical Engineering Inner Mongolia Engineering and Technology Research Center for Catalytic Conversion and Utilization of Carbon Resource Molecules and Inner Mongolia Key Lab of Nanoscience and Nanotechnology Inner Mongolia University 235 West University Street Hohhot 010021 P. R. ChinaAbstract Electrocatalytic nitrogen reduction reaction (NRR) is a promising alternative to the traditional Haber–Bosch process. However, the sluggish kinetics and competitive hydrogen evolution reaction result in poor NH3 yield and low Faradaic efficiency (FE). Herein, single bismuth atoms incorporated hollow titanium nitride nanorods encapsulated in nitrogen‐doped carbon layer (NC) supported on carbon cloth (NC/Bi SAs/TiN/CC) is constructed for electrocatalytic NRR. Impressively, as an integrated electrode, it exhibits a superior ammonia yield rate of 76.15 µg mgcat−1 h−1 (9859 µg μmolBi−1 h−1) at −0.8 V versus RHE and a high FE of 24.60% at −0.5 V versus RHE in 0.1 m Na2SO4 solution, which can retain stable performance in 10 h continuous operation, surpassing the overwhelming majority of reported Bi‐based NRR catalysts. Coupling various characterizations with theory calculations, it is disclosed that the unique monolithic core‐shell configuration with porous structure endows abundant accessible active sites, outstanding charge‐transfer property, and good stability, while the cooperation effect of Bi SAs and TiN can simultaneously promote the hydrogenation of N2 into NH3* on the TiN surface and the desorption of NH3* to release NH3 on the Bi SA sites. These features result in the significant promotion of NRR performance.https://doi.org/10.1002/advs.202104245density functional theory calculationelectrocatalysismonolithic electrodesnitrogen reduction reactionsingle bismuth atoms |
| spellingShingle | Zichao Xi Ke Shi Xuan Xu Peng Jing Baocang Liu Rui Gao Jun Zhang Boosting Nitrogen Reduction Reaction via Electronic Coupling of Atomically Dispersed Bismuth with Titanium Nitride Nanorods Advanced Science density functional theory calculation electrocatalysis monolithic electrodes nitrogen reduction reaction single bismuth atoms |
| title | Boosting Nitrogen Reduction Reaction via Electronic Coupling of Atomically Dispersed Bismuth with Titanium Nitride Nanorods |
| title_full | Boosting Nitrogen Reduction Reaction via Electronic Coupling of Atomically Dispersed Bismuth with Titanium Nitride Nanorods |
| title_fullStr | Boosting Nitrogen Reduction Reaction via Electronic Coupling of Atomically Dispersed Bismuth with Titanium Nitride Nanorods |
| title_full_unstemmed | Boosting Nitrogen Reduction Reaction via Electronic Coupling of Atomically Dispersed Bismuth with Titanium Nitride Nanorods |
| title_short | Boosting Nitrogen Reduction Reaction via Electronic Coupling of Atomically Dispersed Bismuth with Titanium Nitride Nanorods |
| title_sort | boosting nitrogen reduction reaction via electronic coupling of atomically dispersed bismuth with titanium nitride nanorods |
| topic | density functional theory calculation electrocatalysis monolithic electrodes nitrogen reduction reaction single bismuth atoms |
| url | https://doi.org/10.1002/advs.202104245 |
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