Regulating the coordination environment of Ru single-atom catalysts and unravelling the reaction path of acetylene hydrochlorination
In this work, DFT calculations were used firstly to simulate the nitrogen coordinated metal single-atom catalysts (M-Nx SACs, M = Hg, Cu, Au, and Ru) to predict their catalytic activities in acetylene hydrochlorination. The DFT results showed that Ru-Nx SACs had the best catalytic performance among...
| Main Authors: | , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
KeAi Communications Co., Ltd.
2023-08-01
|
| Series: | Green Energy & Environment |
| Subjects: | |
| Online Access: | http://www.sciencedirect.com/science/article/pii/S2468025722000061 |
| _version_ | 1827906354275155968 |
|---|---|
| author | Yang Yang Chaoyue Zhao Xianliang Qiao Qingxin Guan Wei Li |
| author_facet | Yang Yang Chaoyue Zhao Xianliang Qiao Qingxin Guan Wei Li |
| author_sort | Yang Yang |
| collection | DOAJ |
| description | In this work, DFT calculations were used firstly to simulate the nitrogen coordinated metal single-atom catalysts (M-Nx SACs, M = Hg, Cu, Au, and Ru) to predict their catalytic activities in acetylene hydrochlorination. The DFT results showed that Ru-Nx SACs had the best catalytic performance among the four catalysts, and Ru-Nx SACs could effectively inhibit the reduction of ruthenium cation. To verify the DFT results, Ru-Nx SACs were fabricated by pyrolyzing MOFs in-situ spatially confined metal precursors. The N coordination environment could be controlled by changing the pyrolysis temperature. Catalytic performance tests indicated that low N coordination number (Ru–N2, Ru–N3) exhibited excellent catalytic activity and stability compared to RuCl3 catalyst. DFT calculations further revealed that Ru–N2 and Ru–N3 had a tendency to activate HCl at the first step of reaction, whereas Ru–N4 tended to activate C2H2. These findings will serve as a reference for the design and control of metal active sites. |
| first_indexed | 2024-03-13T00:55:16Z |
| format | Article |
| id | doaj.art-80af68f63ea54308bcb2826f88f932b6 |
| institution | Directory Open Access Journal |
| issn | 2468-0257 |
| language | English |
| last_indexed | 2024-03-13T00:55:16Z |
| publishDate | 2023-08-01 |
| publisher | KeAi Communications Co., Ltd. |
| record_format | Article |
| series | Green Energy & Environment |
| spelling | doaj.art-80af68f63ea54308bcb2826f88f932b62023-07-07T04:27:39ZengKeAi Communications Co., Ltd.Green Energy & Environment2468-02572023-08-018411411153Regulating the coordination environment of Ru single-atom catalysts and unravelling the reaction path of acetylene hydrochlorinationYang Yang0Chaoyue Zhao1Xianliang Qiao2Qingxin Guan3Wei Li4State Key Laboratory of Elemento-Organic Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, No. 94 Weijin Road, Tianjin, 300071, ChinaState Key Laboratory of Elemento-Organic Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, No. 94 Weijin Road, Tianjin, 300071, ChinaState Key Laboratory of Elemento-Organic Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, No. 94 Weijin Road, Tianjin, 300071, ChinaCorresponding authors.; State Key Laboratory of Elemento-Organic Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, No. 94 Weijin Road, Tianjin, 300071, ChinaCorresponding authors.; State Key Laboratory of Elemento-Organic Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, No. 94 Weijin Road, Tianjin, 300071, ChinaIn this work, DFT calculations were used firstly to simulate the nitrogen coordinated metal single-atom catalysts (M-Nx SACs, M = Hg, Cu, Au, and Ru) to predict their catalytic activities in acetylene hydrochlorination. The DFT results showed that Ru-Nx SACs had the best catalytic performance among the four catalysts, and Ru-Nx SACs could effectively inhibit the reduction of ruthenium cation. To verify the DFT results, Ru-Nx SACs were fabricated by pyrolyzing MOFs in-situ spatially confined metal precursors. The N coordination environment could be controlled by changing the pyrolysis temperature. Catalytic performance tests indicated that low N coordination number (Ru–N2, Ru–N3) exhibited excellent catalytic activity and stability compared to RuCl3 catalyst. DFT calculations further revealed that Ru–N2 and Ru–N3 had a tendency to activate HCl at the first step of reaction, whereas Ru–N4 tended to activate C2H2. These findings will serve as a reference for the design and control of metal active sites.http://www.sciencedirect.com/science/article/pii/S2468025722000061Single-atom catalystCoordination environmentRu-based catalystDFT calculationsAcetylene hydrochlorination |
| spellingShingle | Yang Yang Chaoyue Zhao Xianliang Qiao Qingxin Guan Wei Li Regulating the coordination environment of Ru single-atom catalysts and unravelling the reaction path of acetylene hydrochlorination Green Energy & Environment Single-atom catalyst Coordination environment Ru-based catalyst DFT calculations Acetylene hydrochlorination |
| title | Regulating the coordination environment of Ru single-atom catalysts and unravelling the reaction path of acetylene hydrochlorination |
| title_full | Regulating the coordination environment of Ru single-atom catalysts and unravelling the reaction path of acetylene hydrochlorination |
| title_fullStr | Regulating the coordination environment of Ru single-atom catalysts and unravelling the reaction path of acetylene hydrochlorination |
| title_full_unstemmed | Regulating the coordination environment of Ru single-atom catalysts and unravelling the reaction path of acetylene hydrochlorination |
| title_short | Regulating the coordination environment of Ru single-atom catalysts and unravelling the reaction path of acetylene hydrochlorination |
| title_sort | regulating the coordination environment of ru single atom catalysts and unravelling the reaction path of acetylene hydrochlorination |
| topic | Single-atom catalyst Coordination environment Ru-based catalyst DFT calculations Acetylene hydrochlorination |
| url | http://www.sciencedirect.com/science/article/pii/S2468025722000061 |
| work_keys_str_mv | AT yangyang regulatingthecoordinationenvironmentofrusingleatomcatalystsandunravellingthereactionpathofacetylenehydrochlorination AT chaoyuezhao regulatingthecoordinationenvironmentofrusingleatomcatalystsandunravellingthereactionpathofacetylenehydrochlorination AT xianliangqiao regulatingthecoordinationenvironmentofrusingleatomcatalystsandunravellingthereactionpathofacetylenehydrochlorination AT qingxinguan regulatingthecoordinationenvironmentofrusingleatomcatalystsandunravellingthereactionpathofacetylenehydrochlorination AT weili regulatingthecoordinationenvironmentofrusingleatomcatalystsandunravellingthereactionpathofacetylenehydrochlorination |