Modulating electronic structure of metal-organic frameworks by introducing atomically dispersed Ru for efficient hydrogen evolution

Developing high-performance electrocatalysts toward hydrogen evolution reaction is important for clean and sustainable hydrogen energy, yet still challenging. Herein, we report a single-atom strategy to construct excellent metal-organic frameworks (MOFs) hydrogen evolution reaction electrocatalyst (...

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Published in	Nature communications Vol. 12; no. 1; pp. 1369 - 8
Main Authors	Sun, Yamei, Xue, Ziqian, Liu, Qinglin, Jia, Yaling, Li, Yinle, Liu, Kang, Lin, Yiyang, Liu, Min, Li, Guangqin, Su, Cheng-Yong
Format	Journal Article
Language	English
Published	London Nature Publishing Group UK 01.03.2021 Nature Publishing Group Nature Portfolio
Subjects	147/135 147/143 639/301/299/886 639/638/298/921 639/925/357 Catalysts Clean energy Density functional theory Dispersion Electrocatalysts Electronic structure Evolution Humanities and Social Sciences Hydrogen Hydrogen evolution reactions Hydrogen-based energy Metal-organic frameworks Metals multidisciplinary Optimization Renewable energy Ruthenium Saline solutions Science Science (multidisciplinary) X ray absorption
Online Access	Get full text
ISSN	2041-1723 2041-1723
DOI	10.1038/s41467-021-21595-5

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Abstract	Developing high-performance electrocatalysts toward hydrogen evolution reaction is important for clean and sustainable hydrogen energy, yet still challenging. Herein, we report a single-atom strategy to construct excellent metal-organic frameworks (MOFs) hydrogen evolution reaction electrocatalyst (NiRu 0.13 -BDC) by introducing atomically dispersed Ru. Significantly, the obtained NiRu 0.13 -BDC exhibits outstanding hydrogen evolution activity in all pH, especially with a low overpotential of 36 mV at a current density of 10 mA cm −2 in 1 M phosphate buffered saline solution, which is comparable to commercial Pt/C. X-ray absorption fine structures and the density functional theory calculations reveal that introducing Ru single-atom can modulate electronic structure of metal center in the MOF, leading to the optimization of binding strength for H 2 O and H*, and the enhancement of HER performance. This work establishes single-atom strategy as an efficient approach to modulate electronic structure of MOFs for catalyst design. Developing high-performance, neutral-media H 2 -evolution electrocatalysts is important for clean and sustainable hydrogen energy, yet rare, expensive elements are most active. Here, authors show that metal-organic frameworks modified with single ruthenium atoms as high-performances catalysts.
AbstractList	Developing high-performance electrocatalysts toward hydrogen evolution reaction is important for clean and sustainable hydrogen energy, yet still challenging. Herein, we report a single-atom strategy to construct excellent metal-organic frameworks (MOFs) hydrogen evolution reaction electrocatalyst (NiRu0.13-BDC) by introducing atomically dispersed Ru. Significantly, the obtained NiRu0.13-BDC exhibits outstanding hydrogen evolution activity in all pH, especially with a low overpotential of 36 mV at a current density of 10 mA cm-2 in 1 M phosphate buffered saline solution, which is comparable to commercial Pt/C. X-ray absorption fine structures and the density functional theory calculations reveal that introducing Ru single-atom can modulate electronic structure of metal center in the MOF, leading to the optimization of binding strength for H2O and H, and the enhancement of HER performance. This work establishes single-atom strategy as an efficient approach to modulate electronic structure of MOFs for catalyst design.Developing high-performance electrocatalysts toward hydrogen evolution reaction is important for clean and sustainable hydrogen energy, yet still challenging. Herein, we report a single-atom strategy to construct excellent metal-organic frameworks (MOFs) hydrogen evolution reaction electrocatalyst (NiRu0.13-BDC) by introducing atomically dispersed Ru. Significantly, the obtained NiRu0.13-BDC exhibits outstanding hydrogen evolution activity in all pH, especially with a low overpotential of 36 mV at a current density of 10 mA cm-2 in 1 M phosphate buffered saline solution, which is comparable to commercial Pt/C. X-ray absorption fine structures and the density functional theory calculations reveal that introducing Ru single-atom can modulate electronic structure of metal center in the MOF, leading to the optimization of binding strength for H2O and H, and the enhancement of HER performance. This work establishes single-atom strategy as an efficient approach to modulate electronic structure of MOFs for catalyst design. Developing high-performance electrocatalysts toward hydrogen evolution reaction is important for clean and sustainable hydrogen energy, yet still challenging. Herein, we report a single-atom strategy to construct excellent metal-organic frameworks (MOFs) hydrogen evolution reaction electrocatalyst (NiRu0.13-BDC) by introducing atomically dispersed Ru. Significantly, the obtained NiRu0.13-BDC exhibits outstanding hydrogen evolution activity in all pH, especially with a low overpotential of 36 mV at a current density of 10 mA cm−2 in 1 M phosphate buffered saline solution, which is comparable to commercial Pt/C. X-ray absorption fine structures and the density functional theory calculations reveal that introducing Ru single-atom can modulate electronic structure of metal center in the MOF, leading to the optimization of binding strength for H2O and H, and the enhancement of HER performance. This work establishes single-atom strategy as an efficient approach to modulate electronic structure of MOFs for catalyst design.Developing high-performance, neutral-media H2-evolution electrocatalysts is important for clean and sustainable hydrogen energy, yet rare, expensive elements are most active. Here, authors show that metal-organic frameworks modified with single ruthenium atoms as high-performances catalysts. Developing high-performance electrocatalysts toward hydrogen evolution reaction is important for clean and sustainable hydrogen energy, yet still challenging. Herein, we report a single-atom strategy to construct excellent metal-organic frameworks (MOFs) hydrogen evolution reaction electrocatalyst (NiRu -BDC) by introducing atomically dispersed Ru. Significantly, the obtained NiRu -BDC exhibits outstanding hydrogen evolution activity in all pH, especially with a low overpotential of 36 mV at a current density of 10 mA cm in 1 M phosphate buffered saline solution, which is comparable to commercial Pt/C. X-ray absorption fine structures and the density functional theory calculations reveal that introducing Ru single-atom can modulate electronic structure of metal center in the MOF, leading to the optimization of binding strength for H O and H, and the enhancement of HER performance. This work establishes single-atom strategy as an efficient approach to modulate electronic structure of MOFs for catalyst design. Developing high-performance, neutral-media H2-evolution electrocatalysts is important for clean and sustainable hydrogen energy, yet rare, expensive elements are most active. Here, authors show that metal-organic frameworks modified with single ruthenium atoms as high-performances catalysts. Developing high-performance electrocatalysts toward hydrogen evolution reaction is important for clean and sustainable hydrogen energy, yet still challenging. Herein, we report a single-atom strategy to construct excellent metal-organic frameworks (MOFs) hydrogen evolution reaction electrocatalyst (NiRu 0.13 -BDC) by introducing atomically dispersed Ru. Significantly, the obtained NiRu 0.13 -BDC exhibits outstanding hydrogen evolution activity in all pH, especially with a low overpotential of 36 mV at a current density of 10 mA cm −2 in 1 M phosphate buffered saline solution, which is comparable to commercial Pt/C. X-ray absorption fine structures and the density functional theory calculations reveal that introducing Ru single-atom can modulate electronic structure of metal center in the MOF, leading to the optimization of binding strength for H 2 O and H, and the enhancement of HER performance. This work establishes single-atom strategy as an efficient approach to modulate electronic structure of MOFs for catalyst design. Developing high-performance, neutral-media H 2 -evolution electrocatalysts is important for clean and sustainable hydrogen energy, yet rare, expensive elements are most active. Here, authors show that metal-organic frameworks modified with single ruthenium atoms as high-performances catalysts. Developing high-performance electrocatalysts toward hydrogen evolution reaction is important for clean and sustainable hydrogen energy, yet still challenging. Herein, we report a single-atom strategy to construct excellent metal-organic frameworks (MOFs) hydrogen evolution reaction electrocatalyst (NiRu 0.13 -BDC) by introducing atomically dispersed Ru. Significantly, the obtained NiRu 0.13 -BDC exhibits outstanding hydrogen evolution activity in all pH, especially with a low overpotential of 36 mV at a current density of 10 mA cm −2 in 1 M phosphate buffered saline solution, which is comparable to commercial Pt/C. X-ray absorption fine structures and the density functional theory calculations reveal that introducing Ru single-atom can modulate electronic structure of metal center in the MOF, leading to the optimization of binding strength for H 2 O and H, and the enhancement of HER performance. This work establishes single-atom strategy as an efficient approach to modulate electronic structure of MOFs for catalyst design.
ArticleNumber	1369
Author	Lin, Yiyang Sun, Yamei Liu, Qinglin Li, Guangqin Su, Cheng-Yong Li, Yinle Xue, Ziqian Jia, Yaling Liu, Kang Liu, Min
Author_xml	– sequence: 1 givenname: Yamei surname: Sun fullname: Sun, Yamei organization: MOE Laboratory of Bioinorganic and Synthetic Chemistry, Lehn Institute of Functional Materials, School of Chemistry, Sun Yat-Sen University – sequence: 2 givenname: Ziqian surname: Xue fullname: Xue, Ziqian organization: MOE Laboratory of Bioinorganic and Synthetic Chemistry, Lehn Institute of Functional Materials, School of Chemistry, Sun Yat-Sen University – sequence: 3 givenname: Qinglin surname: Liu fullname: Liu, Qinglin organization: MOE Laboratory of Bioinorganic and Synthetic Chemistry, Lehn Institute of Functional Materials, School of Chemistry, Sun Yat-Sen University – sequence: 4 givenname: Yaling surname: Jia fullname: Jia, Yaling organization: MOE Laboratory of Bioinorganic and Synthetic Chemistry, Lehn Institute of Functional Materials, School of Chemistry, Sun Yat-Sen University – sequence: 5 givenname: Yinle surname: Li fullname: Li, Yinle organization: MOE Laboratory of Bioinorganic and Synthetic Chemistry, Lehn Institute of Functional Materials, School of Chemistry, Sun Yat-Sen University – sequence: 6 givenname: Kang surname: Liu fullname: Liu, Kang organization: School of Physics and Electronics, Central South University – sequence: 7 givenname: Yiyang surname: Lin fullname: Lin, Yiyang organization: School of Physics and Electronics, Central South University – sequence: 8 givenname: Min orcidid: 0000-0002-9007-4817 surname: Liu fullname: Liu, Min organization: School of Physics and Electronics, Central South University – sequence: 9 givenname: Guangqin surname: Li fullname: Li, Guangqin email: liguangqin@mail.sysu.edu.cn organization: MOE Laboratory of Bioinorganic and Synthetic Chemistry, Lehn Institute of Functional Materials, School of Chemistry, Sun Yat-Sen University – sequence: 10 givenname: Cheng-Yong orcidid: 0000-0003-3604-7858 surname: Su fullname: Su, Cheng-Yong organization: MOE Laboratory of Bioinorganic and Synthetic Chemistry, Lehn Institute of Functional Materials, School of Chemistry, Sun Yat-Sen University
BackLink	https://www.ncbi.nlm.nih.gov/pubmed/33649349$$D View this record in MEDLINE/PubMed
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Snippet	Developing high-performance electrocatalysts toward hydrogen evolution reaction is important for clean and sustainable hydrogen energy, yet still challenging.... Developing high-performance, neutral-media H2-evolution electrocatalysts is important for clean and sustainable hydrogen energy, yet rare, expensive elements...
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SubjectTerms	147/135 147/143 639/301/299/886 639/638/298/921 639/925/357 Catalysts Clean energy Density functional theory Dispersion Electrocatalysts Electronic structure Evolution Humanities and Social Sciences Hydrogen Hydrogen evolution reactions Hydrogen-based energy Metal-organic frameworks Metals multidisciplinary Optimization Renewable energy Ruthenium Saline solutions Science Science (multidisciplinary) X ray absorption
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Title	Modulating electronic structure of metal-organic frameworks by introducing atomically dispersed Ru for efficient hydrogen evolution
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