Rational Design of Three Dimensional Hollow Heterojunctions for Efficient Photocatalytic Hydrogen Evolution Applications
The efficiency of photocatalytic hydrogen evolution is currently limited by poor light adsorption, rapid recombination of photogenerated carriers, and ineffective surface reaction rate. Although heterojunctions with innovative morphologies and structures can strengthen built‐in electric fields and m...
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| Published in | Advanced science Vol. 11; no. 13; pp. e2309293 - n/a |
|---|---|
| Main Authors | , , , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
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Germany
John Wiley & Sons, Inc
01.04.2024
John Wiley and Sons Inc Wiley |
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| Abstract | The efficiency of photocatalytic hydrogen evolution is currently limited by poor light adsorption, rapid recombination of photogenerated carriers, and ineffective surface reaction rate. Although heterojunctions with innovative morphologies and structures can strengthen built‐in electric fields and maximize the separation of photogenerated charges. However, how to rational design of novel multidimensional structures to simultaneously improve the above three bottleneck problems is still a research imperative. Herein, a unique Cu2O─S@graphene oxide (GO)@Zn0.67Cd0.33S Three dimensional (3D) hollow heterostructure is designed and synthesized, which greatly extends the carrier lifetime and effectively promotes the separation of photogenerated charges. The H2 production rate reached 48.5 mmol g−1 h−1 under visible light after loading Ni2+ on the heterojunction surface, which is 97 times higher than that of pure Zn0.67Cd0.33S nanospheres. Furthermore, the H2 production rate can reach 77.3 mmol g−1 h−1 without cooling, verifying the effectiveness of the photothermal effect. Meanwhile, in situ characterization and density flooding theory calculations reveal the efficient charge transfer at the p‐n 3D hollow heterojunction interface. This study not only reveals the detailed mechanism of photocatalytic hydrogen evolution in depth but also rationalizes the construction of superior 3D hollow heterojunctions, thus providing a universal strategy for the materials‐by‐design of high‐performance heterojunctions.
Herein, a unique Cu2O─S@graphene oxide (GO)@Zn0.67Cd0.33S 3D hollow heterostructure is designed to realize the spatial separation and effective transfer of photogenerated charges. This study not only reveals the detailed mechanism of photocatalytic hydrogen evolution in depth through in situ characterization and theoretical calculations but also provides a universal strategy for the rational construction of excellent hollow heterojunctions. |
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| AbstractList | Abstract The efficiency of photocatalytic hydrogen evolution is currently limited by poor light adsorption, rapid recombination of photogenerated carriers, and ineffective surface reaction rate. Although heterojunctions with innovative morphologies and structures can strengthen built‐in electric fields and maximize the separation of photogenerated charges. However, how to rational design of novel multidimensional structures to simultaneously improve the above three bottleneck problems is still a research imperative. Herein, a unique Cu2O─S@graphene oxide (GO)@Zn0.67Cd0.33S Three dimensional (3D) hollow heterostructure is designed and synthesized, which greatly extends the carrier lifetime and effectively promotes the separation of photogenerated charges. The H2 production rate reached 48.5 mmol g−1 h−1 under visible light after loading Ni2+ on the heterojunction surface, which is 97 times higher than that of pure Zn0.67Cd0.33S nanospheres. Furthermore, the H2 production rate can reach 77.3 mmol g−1 h−1 without cooling, verifying the effectiveness of the photothermal effect. Meanwhile, in situ characterization and density flooding theory calculations reveal the efficient charge transfer at the p‐n 3D hollow heterojunction interface. This study not only reveals the detailed mechanism of photocatalytic hydrogen evolution in depth but also rationalizes the construction of superior 3D hollow heterojunctions, thus providing a universal strategy for the materials‐by‐design of high‐performance heterojunctions. The efficiency of photocatalytic hydrogen evolution is currently limited by poor light adsorption, rapid recombination of photogenerated carriers, and ineffective surface reaction rate. Although heterojunctions with innovative morphologies and structures can strengthen built‐in electric fields and maximize the separation of photogenerated charges. However, how to rational design of novel multidimensional structures to simultaneously improve the above three bottleneck problems is still a research imperative. Herein, a unique Cu 2 O─S@graphene oxide (GO)@Zn 0.67 Cd 0.33 S Three dimensional (3D) hollow heterostructure is designed and synthesized, which greatly extends the carrier lifetime and effectively promotes the separation of photogenerated charges. The H 2 production rate reached 48.5 mmol g −1 h −1 under visible light after loading Ni 2+ on the heterojunction surface, which is 97 times higher than that of pure Zn 0.67 Cd 0.33 S nanospheres. Furthermore, the H 2 production rate can reach 77.3 mmol g −1 h −1 without cooling, verifying the effectiveness of the photothermal effect. Meanwhile, in situ characterization and density flooding theory calculations reveal the efficient charge transfer at the p‐n 3D hollow heterojunction interface. This study not only reveals the detailed mechanism of photocatalytic hydrogen evolution in depth but also rationalizes the construction of superior 3D hollow heterojunctions, thus providing a universal strategy for the materials‐by‐design of high‐performance heterojunctions. Herein, a unique Cu 2 O─S@graphene oxide (GO)@Zn 0.67 Cd 0.33 S 3D hollow heterostructure is designed to realize the spatial separation and effective transfer of photogenerated charges. This study not only reveals the detailed mechanism of photocatalytic hydrogen evolution in depth through in situ characterization and theoretical calculations but also provides a universal strategy for the rational construction of excellent hollow heterojunctions. The efficiency of photocatalytic hydrogen evolution is currently limited by poor light adsorption, rapid recombination of photogenerated carriers, and ineffective surface reaction rate. Although heterojunctions with innovative morphologies and structures can strengthen built-in electric fields and maximize the separation of photogenerated charges. However, how to rational design of novel multidimensional structures to simultaneously improve the above three bottleneck problems is still a research imperative. Herein, a unique Cu2O─S@graphene oxide (GO)@Zn0.67Cd0.33S Three dimensional (3D) hollow heterostructure is designed and synthesized, which greatly extends the carrier lifetime and effectively promotes the separation of photogenerated charges. The H2 production rate reached 48.5 mmol g−1 h−1 under visible light after loading Ni2+ on the heterojunction surface, which is 97 times higher than that of pure Zn0.67Cd0.33S nanospheres. Furthermore, the H2 production rate can reach 77.3 mmol g−1 h−1 without cooling, verifying the effectiveness of the photothermal effect. Meanwhile, in situ characterization and density flooding theory calculations reveal the efficient charge transfer at the p-n 3D hollow heterojunction interface. This study not only reveals the detailed mechanism of photocatalytic hydrogen evolution in depth but also rationalizes the construction of superior 3D hollow heterojunctions, thus providing a universal strategy for the materials-by-design of high-performance heterojunctions. The efficiency of photocatalytic hydrogen evolution is currently limited by poor light adsorption, rapid recombination of photogenerated carriers, and ineffective surface reaction rate. Although heterojunctions with innovative morphologies and structures can strengthen built-in electric fields and maximize the separation of photogenerated charges. However, how to rational design of novel multidimensional structures to simultaneously improve the above three bottleneck problems is still a research imperative. Herein, a unique Cu2O─S@graphene oxide (GO)@Zn0.67Cd0.33S Three dimensional (3D) hollow heterostructure is designed and synthesized, which greatly extends the carrier lifetime and effectively promotes the separation of photogenerated charges. The H2 production rate reached 48.5 mmol g-1 h-1 under visible light after loading Ni2+ on the heterojunction surface, which is 97 times higher than that of pure Zn0.67Cd0.33S nanospheres. Furthermore, the H2 production rate can reach 77.3 mmol g-1 h-1 without cooling, verifying the effectiveness of the photothermal effect. Meanwhile, in situ characterization and density flooding theory calculations reveal the efficient charge transfer at the p-n 3D hollow heterojunction interface. This study not only reveals the detailed mechanism of photocatalytic hydrogen evolution in depth but also rationalizes the construction of superior 3D hollow heterojunctions, thus providing a universal strategy for the materials-by-design of high-performance heterojunctions.The efficiency of photocatalytic hydrogen evolution is currently limited by poor light adsorption, rapid recombination of photogenerated carriers, and ineffective surface reaction rate. Although heterojunctions with innovative morphologies and structures can strengthen built-in electric fields and maximize the separation of photogenerated charges. However, how to rational design of novel multidimensional structures to simultaneously improve the above three bottleneck problems is still a research imperative. Herein, a unique Cu2O─S@graphene oxide (GO)@Zn0.67Cd0.33S Three dimensional (3D) hollow heterostructure is designed and synthesized, which greatly extends the carrier lifetime and effectively promotes the separation of photogenerated charges. The H2 production rate reached 48.5 mmol g-1 h-1 under visible light after loading Ni2+ on the heterojunction surface, which is 97 times higher than that of pure Zn0.67Cd0.33S nanospheres. Furthermore, the H2 production rate can reach 77.3 mmol g-1 h-1 without cooling, verifying the effectiveness of the photothermal effect. Meanwhile, in situ characterization and density flooding theory calculations reveal the efficient charge transfer at the p-n 3D hollow heterojunction interface. This study not only reveals the detailed mechanism of photocatalytic hydrogen evolution in depth but also rationalizes the construction of superior 3D hollow heterojunctions, thus providing a universal strategy for the materials-by-design of high-performance heterojunctions. The efficiency of photocatalytic hydrogen evolution is currently limited by poor light adsorption, rapid recombination of photogenerated carriers, and ineffective surface reaction rate. Although heterojunctions with innovative morphologies and structures can strengthen built‐in electric fields and maximize the separation of photogenerated charges. However, how to rational design of novel multidimensional structures to simultaneously improve the above three bottleneck problems is still a research imperative. Herein, a unique Cu2O─S@graphene oxide (GO)@Zn0.67Cd0.33S Three dimensional (3D) hollow heterostructure is designed and synthesized, which greatly extends the carrier lifetime and effectively promotes the separation of photogenerated charges. The H2 production rate reached 48.5 mmol g−1 h−1 under visible light after loading Ni2+ on the heterojunction surface, which is 97 times higher than that of pure Zn0.67Cd0.33S nanospheres. Furthermore, the H2 production rate can reach 77.3 mmol g−1 h−1 without cooling, verifying the effectiveness of the photothermal effect. Meanwhile, in situ characterization and density flooding theory calculations reveal the efficient charge transfer at the p‐n 3D hollow heterojunction interface. This study not only reveals the detailed mechanism of photocatalytic hydrogen evolution in depth but also rationalizes the construction of superior 3D hollow heterojunctions, thus providing a universal strategy for the materials‐by‐design of high‐performance heterojunctions. Herein, a unique Cu2O─S@graphene oxide (GO)@Zn0.67Cd0.33S 3D hollow heterostructure is designed to realize the spatial separation and effective transfer of photogenerated charges. This study not only reveals the detailed mechanism of photocatalytic hydrogen evolution in depth through in situ characterization and theoretical calculations but also provides a universal strategy for the rational construction of excellent hollow heterojunctions. The efficiency of photocatalytic hydrogen evolution is currently limited by poor light adsorption, rapid recombination of photogenerated carriers, and ineffective surface reaction rate. Although heterojunctions with innovative morphologies and structures can strengthen built-in electric fields and maximize the separation of photogenerated charges. However, how to rational design of novel multidimensional structures to simultaneously improve the above three bottleneck problems is still a research imperative. Herein, a unique Cu O─S@graphene oxide (GO)@Zn Cd S Three dimensional (3D) hollow heterostructure is designed and synthesized, which greatly extends the carrier lifetime and effectively promotes the separation of photogenerated charges. The H production rate reached 48.5 mmol g h under visible light after loading Ni on the heterojunction surface, which is 97 times higher than that of pure Zn Cd S nanospheres. Furthermore, the H production rate can reach 77.3 mmol g h without cooling, verifying the effectiveness of the photothermal effect. Meanwhile, in situ characterization and density flooding theory calculations reveal the efficient charge transfer at the p-n 3D hollow heterojunction interface. This study not only reveals the detailed mechanism of photocatalytic hydrogen evolution in depth but also rationalizes the construction of superior 3D hollow heterojunctions, thus providing a universal strategy for the materials-by-design of high-performance heterojunctions. The efficiency of photocatalytic hydrogen evolution is currently limited by poor light adsorption, rapid recombination of photogenerated carriers, and ineffective surface reaction rate. Although heterojunctions with innovative morphologies and structures can strengthen built‐in electric fields and maximize the separation of photogenerated charges. However, how to rational design of novel multidimensional structures to simultaneously improve the above three bottleneck problems is still a research imperative. Herein, a unique Cu 2 O─S@graphene oxide (GO)@Zn 0.67 Cd 0.33 S Three dimensional (3D) hollow heterostructure is designed and synthesized, which greatly extends the carrier lifetime and effectively promotes the separation of photogenerated charges. The H 2 production rate reached 48.5 mmol g −1 h −1 under visible light after loading Ni 2+ on the heterojunction surface, which is 97 times higher than that of pure Zn 0.67 Cd 0.33 S nanospheres. Furthermore, the H 2 production rate can reach 77.3 mmol g −1 h −1 without cooling, verifying the effectiveness of the photothermal effect. Meanwhile, in situ characterization and density flooding theory calculations reveal the efficient charge transfer at the p‐n 3D hollow heterojunction interface. This study not only reveals the detailed mechanism of photocatalytic hydrogen evolution in depth but also rationalizes the construction of superior 3D hollow heterojunctions, thus providing a universal strategy for the materials‐by‐design of high‐performance heterojunctions. |
| Author | Liu, Gang Xu, Zhikun Zhao, Chenchen Zhang, Bingke Pan, Jingwen Wang, Jinzhong Zeng, Zhi Jiao, Shujie Liu, Sihang Liu, Donghao Zhao, Liancheng Wu, Donghai Wang, Dongbo Fang, Xuan Cao, Jiamu |
| AuthorAffiliation | 2 Henan Key Laboratory of Nanocomposites and Applications Huanghe Science and Technology College Institute of Nanostructured Functional Materials Zhengzhou 450006 China 4 State Key Lab High Power Semicond Lasers Changchun University Science and Technology, Sch Sci Changchun 130022 China 1 School of Materials Science and Engineering Harbin Institute of Technology Harbin 150001 China 3 School of Astronautics Harbin Institute of Technology Harbin 150001 China 6 Guangdong University of Petrochemical Technology Maoming 525000 China 5 Center for High Pressure Science and Technology Advanced Research Shanghai 201203 China |
| AuthorAffiliation_xml | – name: 6 Guangdong University of Petrochemical Technology Maoming 525000 China – name: 1 School of Materials Science and Engineering Harbin Institute of Technology Harbin 150001 China – name: 4 State Key Lab High Power Semicond Lasers Changchun University Science and Technology, Sch Sci Changchun 130022 China – name: 2 Henan Key Laboratory of Nanocomposites and Applications Huanghe Science and Technology College Institute of Nanostructured Functional Materials Zhengzhou 450006 China – name: 5 Center for High Pressure Science and Technology Advanced Research Shanghai 201203 China – name: 3 School of Astronautics Harbin Institute of Technology Harbin 150001 China |
| Author_xml | – sequence: 1 givenname: Jingwen surname: Pan fullname: Pan, Jingwen organization: Harbin Institute of Technology – sequence: 2 givenname: Dongbo orcidid: 0000-0001-6058-9660 surname: Wang fullname: Wang, Dongbo email: wangdongbo@hit.edu.cn organization: Harbin Institute of Technology – sequence: 3 givenname: Donghai surname: Wu fullname: Wu, Donghai email: donghaiwu@hhstu.edu.cn organization: Institute of Nanostructured Functional Materials – sequence: 4 givenname: Jiamu surname: Cao fullname: Cao, Jiamu email: caojiamu@hit.edu.cn organization: Harbin Institute of Technology – sequence: 5 givenname: Xuan surname: Fang fullname: Fang, Xuan email: fangx@cust.edu.cn organization: Changchun University Science and Technology, Sch Sci – sequence: 6 givenname: Chenchen surname: Zhao fullname: Zhao, Chenchen organization: Harbin Institute of Technology – sequence: 7 givenname: Zhi surname: Zeng fullname: Zeng, Zhi organization: Harbin Institute of Technology – sequence: 8 givenname: Bingke surname: Zhang fullname: Zhang, Bingke organization: Harbin Institute of Technology – sequence: 9 givenname: Donghao surname: Liu fullname: Liu, Donghao organization: Harbin Institute of Technology – sequence: 10 givenname: Sihang surname: Liu fullname: Liu, Sihang organization: Harbin Institute of Technology – sequence: 11 givenname: Gang surname: Liu fullname: Liu, Gang email: liugang@hpstar.ac.cn organization: Center for High Pressure Science and Technology Advanced Research – sequence: 12 givenname: Shujie surname: Jiao fullname: Jiao, Shujie organization: Harbin Institute of Technology – sequence: 13 givenname: Zhikun surname: Xu fullname: Xu, Zhikun email: xuzhikunnano@163.com organization: Guangdong University of Petrochemical Technology – sequence: 14 givenname: Liancheng surname: Zhao fullname: Zhao, Liancheng email: lczhao@hit.edu.cn organization: Harbin Institute of Technology – sequence: 15 givenname: Jinzhong surname: Wang fullname: Wang, Jinzhong email: jinzhong_wang@hit.edu.cn organization: Harbin Institute of Technology |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/38258489$$D View this record in MEDLINE/PubMed |
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| Snippet | The efficiency of photocatalytic hydrogen evolution is currently limited by poor light adsorption, rapid recombination of photogenerated carriers, and... Abstract The efficiency of photocatalytic hydrogen evolution is currently limited by poor light adsorption, rapid recombination of photogenerated carriers, and... |
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| SubjectTerms | 3D hollow heterojunctions Alternative energy sources built‐in electric field Carbon Cu2O─S@GO@Zn0.67Cd0.33S Efficiency Electric fields Energy resources Graphene Hydrogen Interfaces Light Photocatalysis photothermal effect Solar energy Solid solutions |
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| Title | Rational Design of Three Dimensional Hollow Heterojunctions for Efficient Photocatalytic Hydrogen Evolution Applications |
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