Oxygen Functionalization-Induced Charging Effect on Boron Active Sites for High-Yield Electrocatalytic NH3 Production
Abstract Ammonia has been recognized as the future renewable energy fuel because of its wide-ranging applications in H2 storage and transportation sector. In order to avoid the environmentally hazardous Haber–Bosch process, recently, the third-generation ambient ammonia synthesis has drawn phenomena...
| Main Authors: | , , , |
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| Format: | Article |
| Language: | English |
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SpringerOpen
2022-11-01
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| Series: | Nano-Micro Letters |
| Subjects: | |
| Online Access: | https://doi.org/10.1007/s40820-022-00966-7 |
| _version_ | 1797984610226798592 |
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| author | Ashmita Biswas Samadhan Kapse Ranjit Thapa Ramendra Sundar Dey |
| author_facet | Ashmita Biswas Samadhan Kapse Ranjit Thapa Ramendra Sundar Dey |
| author_sort | Ashmita Biswas |
| collection | DOAJ |
| description | Abstract Ammonia has been recognized as the future renewable energy fuel because of its wide-ranging applications in H2 storage and transportation sector. In order to avoid the environmentally hazardous Haber–Bosch process, recently, the third-generation ambient ammonia synthesis has drawn phenomenal attention and thus tremendous efforts are devoted to developing efficient electrocatalysts that would circumvent the bottlenecks of the electrochemical nitrogen reduction reaction (NRR) like competitive hydrogen evolution reaction, poor selectivity of N2 on catalyst surface. Herein, we report the synthesis of an oxygen-functionalized boron carbonitride matrix via a two-step pyrolysis technique. The conductive BNCO(1000) architecture, the compatibility of B-2p z orbital with the N-2p z orbital and the charging effect over B due to the C and O edge-atoms in a pentagon altogether facilitate N2 adsorption on the B edge-active sites. The optimum electrolyte acidity with 0.1 M HCl and the lowered anion crowding effect aid the protonation steps of NRR via an associative alternating pathway, which gives a sufficiently high yield of ammonia (211.5 μg h−1 mgcat −1) on the optimized BNCO(1000) catalyst with a Faradaic efficiency of 34.7% at − 0.1 V vs RHE. This work thus offers a cost-effective electrode material and provides a contemporary idea about reinforcing the charging effect over the secured active sites for NRR by selectively choosing the electrolyte anions and functionalizing the active edges of the BNCO(1000) catalyst. |
| first_indexed | 2024-04-11T07:05:37Z |
| format | Article |
| id | doaj.art-5b13b7fcc4944864b85b4ed33998fc18 |
| institution | Directory Open Access Journal |
| issn | 2311-6706 2150-5551 |
| language | English |
| last_indexed | 2024-04-11T07:05:37Z |
| publishDate | 2022-11-01 |
| publisher | SpringerOpen |
| record_format | Article |
| series | Nano-Micro Letters |
| spelling | doaj.art-5b13b7fcc4944864b85b4ed33998fc182022-12-22T04:38:25ZengSpringerOpenNano-Micro Letters2311-67062150-55512022-11-0114111710.1007/s40820-022-00966-7Oxygen Functionalization-Induced Charging Effect on Boron Active Sites for High-Yield Electrocatalytic NH3 ProductionAshmita Biswas0Samadhan Kapse1Ranjit Thapa2Ramendra Sundar Dey3Institute of Nano Science and Technology (INST)Department of Physics, SRM University–APDepartment of Physics, SRM University–APInstitute of Nano Science and Technology (INST)Abstract Ammonia has been recognized as the future renewable energy fuel because of its wide-ranging applications in H2 storage and transportation sector. In order to avoid the environmentally hazardous Haber–Bosch process, recently, the third-generation ambient ammonia synthesis has drawn phenomenal attention and thus tremendous efforts are devoted to developing efficient electrocatalysts that would circumvent the bottlenecks of the electrochemical nitrogen reduction reaction (NRR) like competitive hydrogen evolution reaction, poor selectivity of N2 on catalyst surface. Herein, we report the synthesis of an oxygen-functionalized boron carbonitride matrix via a two-step pyrolysis technique. The conductive BNCO(1000) architecture, the compatibility of B-2p z orbital with the N-2p z orbital and the charging effect over B due to the C and O edge-atoms in a pentagon altogether facilitate N2 adsorption on the B edge-active sites. The optimum electrolyte acidity with 0.1 M HCl and the lowered anion crowding effect aid the protonation steps of NRR via an associative alternating pathway, which gives a sufficiently high yield of ammonia (211.5 μg h−1 mgcat −1) on the optimized BNCO(1000) catalyst with a Faradaic efficiency of 34.7% at − 0.1 V vs RHE. This work thus offers a cost-effective electrode material and provides a contemporary idea about reinforcing the charging effect over the secured active sites for NRR by selectively choosing the electrolyte anions and functionalizing the active edges of the BNCO(1000) catalyst.https://doi.org/10.1007/s40820-022-00966-7C-doped boron nitrideO-functionalizationDensity-functional theory (DFT)Charging effectNitrogen reduction reactionAmbient ammonia synthesis |
| spellingShingle | Ashmita Biswas Samadhan Kapse Ranjit Thapa Ramendra Sundar Dey Oxygen Functionalization-Induced Charging Effect on Boron Active Sites for High-Yield Electrocatalytic NH3 Production Nano-Micro Letters C-doped boron nitride O-functionalization Density-functional theory (DFT) Charging effect Nitrogen reduction reaction Ambient ammonia synthesis |
| title | Oxygen Functionalization-Induced Charging Effect on Boron Active Sites for High-Yield Electrocatalytic NH3 Production |
| title_full | Oxygen Functionalization-Induced Charging Effect on Boron Active Sites for High-Yield Electrocatalytic NH3 Production |
| title_fullStr | Oxygen Functionalization-Induced Charging Effect on Boron Active Sites for High-Yield Electrocatalytic NH3 Production |
| title_full_unstemmed | Oxygen Functionalization-Induced Charging Effect on Boron Active Sites for High-Yield Electrocatalytic NH3 Production |
| title_short | Oxygen Functionalization-Induced Charging Effect on Boron Active Sites for High-Yield Electrocatalytic NH3 Production |
| title_sort | oxygen functionalization induced charging effect on boron active sites for high yield electrocatalytic nh3 production |
| topic | C-doped boron nitride O-functionalization Density-functional theory (DFT) Charging effect Nitrogen reduction reaction Ambient ammonia synthesis |
| url | https://doi.org/10.1007/s40820-022-00966-7 |
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