A Simple and Effective Principle for a Rational Design of Heterogeneous Catalysts for Dehydrogenation of Formic Acid
Efficient and selective dehydrogenation of formic acid is a key challenge for a fuel‐cell‐based hydrogen economy. Though the development of heterogeneous catalysts has received much progress, their catalytic activity remains insufficient. Moreover, the design principle of such catalysts are still un...
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| Published in | Advanced materials (Weinheim) Vol. 31; no. 15; pp. e1806781 - n/a |
|---|---|
| Main Authors | , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Germany
Wiley Subscription Services, Inc
01.04.2019
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| Online Access | Get full text |
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| Abstract | Efficient and selective dehydrogenation of formic acid is a key challenge for a fuel‐cell‐based hydrogen economy. Though the development of heterogeneous catalysts has received much progress, their catalytic activity remains insufficient. Moreover, the design principle of such catalysts are still unclear. Here, experimental and theoretical studies on a series of mono‐/bi‐metallic nanoparticles supported on a NH2‐N‐rGO substrate are combined for formic acid dehydrogenation where the surface energy of a metal is taken as a relevant indicator for the adsorption ability of the catalyst for guiding catalyst design. The AuPd/NH2‐N‐rGO catalyst shows record catalytic activity by reducing the energy barrier of rate controlling steps of formate adsorption and hydrogen desorption. The obtained excellent results both in experiments and simulations could be extended to other important systems, providing a general guideline to design more efficient catalysts.
A AuPd/NH2‐N‐rGO catalyst shows supreme catalytic performance for the decomposition of formic acid at room temperature, with a turnover frequency (TOF) of 4445.6 h−1. Developments in the experiments and simulations of high‐performance catalysts may promote the practical application of formic acid as a promising hydrogen storage material. |
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| AbstractList | Efficient and selective dehydrogenation of formic acid is a key challenge for a fuel‐cell‐based hydrogen economy. Though the development of heterogeneous catalysts has received much progress, their catalytic activity remains insufficient. Moreover, the design principle of such catalysts are still unclear. Here, experimental and theoretical studies on a series of mono‐/bi‐metallic nanoparticles supported on a NH
2
‐N‐rGO substrate are combined for formic acid dehydrogenation where the surface energy of a metal is taken as a relevant indicator for the adsorption ability of the catalyst for guiding catalyst design. The AuPd/NH
2
‐N‐rGO catalyst shows record catalytic activity by reducing the energy barrier of rate controlling steps of formate adsorption and hydrogen desorption. The obtained excellent results both in experiments and simulations could be extended to other important systems, providing a general guideline to design more efficient catalysts. Efficient and selective dehydrogenation of formic acid is a key challenge for a fuel‐cell‐based hydrogen economy. Though the development of heterogeneous catalysts has received much progress, their catalytic activity remains insufficient. Moreover, the design principle of such catalysts are still unclear. Here, experimental and theoretical studies on a series of mono‐/bi‐metallic nanoparticles supported on a NH2‐N‐rGO substrate are combined for formic acid dehydrogenation where the surface energy of a metal is taken as a relevant indicator for the adsorption ability of the catalyst for guiding catalyst design. The AuPd/NH2‐N‐rGO catalyst shows record catalytic activity by reducing the energy barrier of rate controlling steps of formate adsorption and hydrogen desorption. The obtained excellent results both in experiments and simulations could be extended to other important systems, providing a general guideline to design more efficient catalysts. Efficient and selective dehydrogenation of formic acid is a key challenge for a fuel-cell-based hydrogen economy. Though the development of heterogeneous catalysts has received much progress, their catalytic activity remains insufficient. Moreover, the design principle of such catalysts are still unclear. Here, experimental and theoretical studies on a series of mono-/bi-metallic nanoparticles supported on a NH2 -N-rGO substrate are combined for formic acid dehydrogenation where the surface energy of a metal is taken as a relevant indicator for the adsorption ability of the catalyst for guiding catalyst design. The AuPd/NH2 -N-rGO catalyst shows record catalytic activity by reducing the energy barrier of rate controlling steps of formate adsorption and hydrogen desorption. The obtained excellent results both in experiments and simulations could be extended to other important systems, providing a general guideline to design more efficient catalysts.Efficient and selective dehydrogenation of formic acid is a key challenge for a fuel-cell-based hydrogen economy. Though the development of heterogeneous catalysts has received much progress, their catalytic activity remains insufficient. Moreover, the design principle of such catalysts are still unclear. Here, experimental and theoretical studies on a series of mono-/bi-metallic nanoparticles supported on a NH2 -N-rGO substrate are combined for formic acid dehydrogenation where the surface energy of a metal is taken as a relevant indicator for the adsorption ability of the catalyst for guiding catalyst design. The AuPd/NH2 -N-rGO catalyst shows record catalytic activity by reducing the energy barrier of rate controlling steps of formate adsorption and hydrogen desorption. The obtained excellent results both in experiments and simulations could be extended to other important systems, providing a general guideline to design more efficient catalysts. Efficient and selective dehydrogenation of formic acid is a key challenge for a fuel‐cell‐based hydrogen economy. Though the development of heterogeneous catalysts has received much progress, their catalytic activity remains insufficient. Moreover, the design principle of such catalysts are still unclear. Here, experimental and theoretical studies on a series of mono‐/bi‐metallic nanoparticles supported on a NH2‐N‐rGO substrate are combined for formic acid dehydrogenation where the surface energy of a metal is taken as a relevant indicator for the adsorption ability of the catalyst for guiding catalyst design. The AuPd/NH2‐N‐rGO catalyst shows record catalytic activity by reducing the energy barrier of rate controlling steps of formate adsorption and hydrogen desorption. The obtained excellent results both in experiments and simulations could be extended to other important systems, providing a general guideline to design more efficient catalysts. A AuPd/NH2‐N‐rGO catalyst shows supreme catalytic performance for the decomposition of formic acid at room temperature, with a turnover frequency (TOF) of 4445.6 h−1. Developments in the experiments and simulations of high‐performance catalysts may promote the practical application of formic acid as a promising hydrogen storage material. Efficient and selective dehydrogenation of formic acid is a key challenge for a fuel-cell-based hydrogen economy. Though the development of heterogeneous catalysts has received much progress, their catalytic activity remains insufficient. Moreover, the design principle of such catalysts are still unclear. Here, experimental and theoretical studies on a series of mono-/bi-metallic nanoparticles supported on a NH -N-rGO substrate are combined for formic acid dehydrogenation where the surface energy of a metal is taken as a relevant indicator for the adsorption ability of the catalyst for guiding catalyst design. The AuPd/NH -N-rGO catalyst shows record catalytic activity by reducing the energy barrier of rate controlling steps of formate adsorption and hydrogen desorption. The obtained excellent results both in experiments and simulations could be extended to other important systems, providing a general guideline to design more efficient catalysts. |
| Author | Li, Si‐Jia Gu, Lin Zhou, Yi‐Tong Yan, Jun‐Min Kang, Xia Liu, Dong‐Xue Jiang, Qing Zhang, Qing‐Hua |
| Author_xml | – sequence: 1 givenname: Si‐Jia surname: Li fullname: Li, Si‐Jia organization: Jilin University – sequence: 2 givenname: Yi‐Tong surname: Zhou fullname: Zhou, Yi‐Tong organization: Jilin University – sequence: 3 givenname: Xia surname: Kang fullname: Kang, Xia organization: Jilin University – sequence: 4 givenname: Dong‐Xue surname: Liu fullname: Liu, Dong‐Xue organization: Jilin University – sequence: 5 givenname: Lin surname: Gu fullname: Gu, Lin organization: Chinese Academy of Sciences – sequence: 6 givenname: Qing‐Hua surname: Zhang fullname: Zhang, Qing‐Hua organization: Chinese Academy of Sciences – sequence: 7 givenname: Jun‐Min orcidid: 0000-0001-8511-3810 surname: Yan fullname: Yan, Jun‐Min email: junminyan@jlu.edu.cn organization: Jilin University – sequence: 8 givenname: Qing surname: Jiang fullname: Jiang, Qing email: jiangq@jlu.edu.cn organization: Jilin University |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/30803061$$D View this record in MEDLINE/PubMed |
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| Copyright | 2019 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. |
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| Keywords | formic acid DFT calculation dehydrogenation catalyst record activity |
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| Snippet | Efficient and selective dehydrogenation of formic acid is a key challenge for a fuel‐cell‐based hydrogen economy. Though the development of heterogeneous... Efficient and selective dehydrogenation of formic acid is a key challenge for a fuel-cell-based hydrogen economy. Though the development of heterogeneous... |
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| SubjectTerms | Adsorption Catalysis catalyst Catalysts Catalytic activity Dehydrogenation DFT calculation Formic acid Hydrogen-based energy Materials science Nanoparticles record activity Substrates Surface energy |
| Title | A Simple and Effective Principle for a Rational Design of Heterogeneous Catalysts for Dehydrogenation of Formic Acid |
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