Controlling catalytic dehydrogenation of formic acid over low-cost transition metal-substituted AuPd nanoparticles immobilized by functionalized metal–organic frameworks at room temperature

Jia, Chenglong; Gu, Xuehong; Liu, Penglong; Wang, Tianshu; Su, Haiquan

doi:10.1039/c6ta05790j

Cited by 51 publications

(32 citation statements)

References 76 publications

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“…[175] The chemocatalytic measurement is conducted by the injection of formic acid and sodium formate aqueous solution into a flask contained with the catalyst. [175] The chemocatalytic measurement is conducted by the injection of formic acid and sodium formate aqueous solution into a flask contained with the catalyst.…”

Section: Mofs As Supportsmentioning

confidence: 99%

“…In other words, at the current stage of research, the functions of MOFs are primarily the structural directing agents and sources of metals. [175,187] Furthermore, many earlier published works prefer ambiguous qualitative terms (such as "no apparent drop" and "little loss") over quantitative descriptions about the results of stability tests. Therefore, the development of chemocatalytically active MOFs for hydrogen evolution is certainly an interesting and challenging work to be explored in the future.…”

Section: Mof Derivativesmentioning

confidence: 99%

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Metal–Organic Framework Based Catalysts for Hydrogen Evolution

Zhu

Zou

2018

Advanced Energy Materials

408

199

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society is still heavily relying on chemical fuels. Therefore, the essential and realistic approaches to environmental and energy issues remain to be the exploration of clean and sustainable energy sources, in order to meet the ever-increasing energy demand. Thanks to its high energy density and environmental friendliness, hydrogen fuel comes into play as a muchanticipated new energy carrier, which is under intensive studies in the academic field. [4] Furthermore, we are already in the new era witnessing the transformation of hydrogen-powered technologies from science fictions to realities. UK is already in the process of replacing their traditional diesel-powered double decker buses with the hydrogen-powered version, which aims to phase out the former by 2018. [5] China announced its world's first hydrogen-powered tram, which was put into business service in the latter half of 2017. [6] Mercedes-Benz had even started its development of personal hydrogen-powered car, and Toyota had commercialized its hydrogen fuel-cell car branded "Mirai." [7,8] However, one critical issue remains to be the conflict between the hydrogen production efficiency and the demand for the mass distribution of hydrogen-powered technologies.Current industrial hydrogen production methods include coal gasification (followed by water-gas shift reaction), steam reforming, cryogenic distillation, and water splitting. [9] Coal gasification and steam reforming utilize the reaction between conventional fossil fuels and water to produce syngas (primarily CO and H 2 ) or CO 2 and H 2 mixture. However, both reactions require high temperatures (can be over 1000 °C) and pressures, which is an energy intensive process and has strict requirements on infrastructures. [10] The reaction products also need to be further separated to obtain relatively high-concentration of hydrogen. Cryogenic distillation takes the advantage of difference in gas boiling points, which can be applied to separate hydrogen from other gas components in the former two hydrogen production methods. However, cryogenic distillation is also an energy intensive process for low-temperature gas liquification. In comparison, hydrogen evolution reaction (HER) through water splitting is much-favored because of the following three prominent advantages: 1) Water splitting can be carried out at room temperature and ambient pressure, which is less restricted by infrastructure requirements. 2) Oxygen and hydrogen can be produced separately or selectively, which eliminate the need for gas separation. 3) Both the hydrogen source Highly efficient hydrogen evolution reactions (HERs) will determine the mass distributions of hydrogen-powered clean technologies in the future. Metal-organic frameworks (MOFs) are emerging as a class of crystalline porous materials. Along with their derivatives, MOFs have recently been under intense study for their applications in various hydrogen production techniques. MOF-based materials possess unique advantages, such as high specific surface area, crystalline porous str...

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Section: Mofs As Supportsmentioning

confidence: 99%

Section: Mof Derivativesmentioning

confidence: 99%

Metal–Organic Framework Based Catalysts for Hydrogen Evolution

Zhu

Zou

2018

Advanced Energy Materials

408

199

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“…It appears that the presence of ZrO 2 modied the electronic structure of the Pd NPs to generate a more electron-rich surface. 28 The more electron-rich Pd NPs would be expected to promote the dissociation of the O-H bonds of FA molecules and therefore favor the formation of Pdformate intermediates during the initial step of the decomposition reaction. This effect, in turn, would improve the catalytic performance.…”

Section: Resultsmentioning

confidence: 99%

“…23 There have been some reports regarding the application of catalysts prepared with MOFs as carriers in the liquid phase decomposition of FA. [24][25][26][27][28] However, the catalytic performance during FAD is not ideal at present, and so further improvements are required. The use of MOFs as sacricial templates for the preparation of nanocomposite materials by simple pyrolysis is an increasingly attractive catalyst preparation technique.…”

Section: Introductionmentioning

confidence: 99%

Enhanced catalytic activity over palladium supported on ZrO₂@C with NaOH-assisted reduction for decomposition of formic acid

Wang

et al. 2019

RSC Adv.

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“…Alternatively, metal-free catalysts using dialkyborane derivatives achieve 79% FA conversion with TOF = 4.1 h −1 after 19 h [15]. Recent focus has been on generating low-cost process by using non-precious transition metals (Fe, Co, Ni) immobilized on metal-organic frameworks (MOFs) with 100% H 2 selectivity and a TOF value of 347 h −1 [16] Separately, several chemical catalytic reactions routes have been demonstrated to convert CO 2 to FA with application in H 2 production [5]. However, the combination of in-situ CO 2 capture from FA dehydrogenation has not been investigated.…”

Section: Introductionmentioning

confidence: 99%

Sustainable Recycling of Formic Acid by Bio-Catalytic CO2 Capture and Re-Hydrogenation

Zhao

Shanbhag

et al. 2019

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Formic acid (FA) is a promising reservoir for hydrogen storage and distribution. Its dehydrogenation releases CO2 as a by-product, which limits its practical application. A proof of concept for a bio-catalytic system that simultaneously combines the dehydrogenation of formic acid for H2, in-situ capture of CO2 and its re-hydrogenation to reform formic acid is demonstrated. Enzymatic reactions catalyzed by carbonic anhydrase (CA) and formate dehydrogenase (FDH) under ambient condition are applied for in-situ CO2 capture and re-hydrogenation, respectively, to develop a sustainable system. Continuous production of FA from stripped CO2 was achieved at a rate of 40% using FDH combined with sustainable co-factor regeneration achieved by electrochemistry. In this study, the complete cycle of FA dehydrogenation, CO2 capture, and re-hydrogenation of CO2 to FA has been demonstrated in a single system. The proposed bio-catalytic system has the potential to reduce emissions of CO2 during H2 production from FA by effectively using it to recycle FA for continuous energy supply.

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Controlling catalytic dehydrogenation of formic acid over low-cost transition metal-substituted AuPd nanoparticles immobilized by functionalized metal–organic frameworks at room temperature

Abstract: Through tuning the functionalized groups in MIL-101, the low-cost catalyst containing NH2 exhibited remarkably high activity in dehydrogenation of HCOOH.

Cited by 51 publications

References 76 publications

Metal–Organic Framework Based Catalysts for Hydrogen Evolution

Metal–Organic Framework Based Catalysts for Hydrogen Evolution

Enhanced catalytic activity over palladium supported on ZrO₂@C with NaOH-assisted reduction for decomposition of formic acid

Sustainable Recycling of Formic Acid by Bio-Catalytic CO2 Capture and Re-Hydrogenation

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Controlling catalytic dehydrogenation of formic acid over low-cost transition metal-substituted AuPd nanoparticles immobilized by functionalized metal–organic frameworks at room temperature

Abstract: Through tuning the functionalized groups in MIL-101, the low-cost catalyst containing NH2 exhibited remarkably high activity in dehydrogenation of HCOOH.

Cited by 51 publications

References 76 publications

Metal–Organic Framework Based Catalysts for Hydrogen Evolution

Metal–Organic Framework Based Catalysts for Hydrogen Evolution

Enhanced catalytic activity over palladium supported on ZrO2@C with NaOH-assisted reduction for decomposition of formic acid

Sustainable Recycling of Formic Acid by Bio-Catalytic CO2 Capture and Re-Hydrogenation

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Enhanced catalytic activity over palladium supported on ZrO₂@C with NaOH-assisted reduction for decomposition of formic acid