Highly Selective Solar-Driven Methanol from CO<sub>2</sub> by a Photocatalyst/Biocatalyst Integrated System

Yadav, Rajesh K.; Oh, Gyu Hwan; Park, No‐Joong; Kumar, Abhishek; Kong, Ki−jeong; Baeg, Jin‐Ook

doi:10.1021/ja509650r

Cited by 202 publications

(150 citation statements)

References 34 publications

(43 reference statements)

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“…One of the most concerning worldwide problems in the rapidly developing world is the overproduction of the greenhouse gas carbon dioxide led by ever‐increasing worldwide consumption of fossil fuels 65. The perfect solution may be conversion of CO 2 to other useful compounds by using sunlight,66, 67, 68 like what has been done by plants. However efficient catalysts are still in fancy.…”

Section: Edges As Active Sitesmentioning

confidence: 99%

Face the Edges: Catalytic Active Sites of Nanomaterials

Wang

2015

Advanced Science

156

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Edges are special sites in nanomaterials. The atoms residing on the edges have different environments compared to those in other parts of a nanomaterial and, therefore, they may have different properties. Here, recent progress in nanomaterial fields is summarized from the viewpoint of the edges. Typically, edge sites in MoS2 or metals, other than surface atoms, can perform as active centers for catalytic reactions, so the method to enhance performance lies in the optimization of the edge structures. The edges of multicomponent interfaces present even more possibilities to enhance the activities of nanomaterials. Nanoframes and ultrathin nanowires have similarities to conventional edges of nanoparticles, the application of which as catalysts can help to reduce the use of costly materials. Looking beyond this, the edge structures of graphene are also essential for their properties. In short, the edge structure can influence many properties of materials.

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Section: Edges As Active Sitesmentioning

confidence: 99%

Face the Edges: Catalytic Active Sites of Nanomaterials

Wang

2015

Advanced Science

156

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“…As a result, 100 to 1000 mol of CH3OH can be produced from 1 mol NADH, creating the possibility for practical application. More recently, a photocatalyst/biocatalyst integrated system for highly selective methanol production directly from CO2 was reported [42]. The system was obtained by combining a newly developed graphene-based photocatalyst with sequentially coupled enzymes (FDH, FaldDH, and ADH) as depicted in Scheme 4.…”

Section: Conversion Of Co2 To Methanementioning

confidence: 99%

“…Scheme 4. Schematic illustration of the photocatalyst/biocatalyst integrated system for producing methanol from CO 2 [42].…”

Section: Conversion Of Co2 To Methanementioning

confidence: 99%

Recent Progress and Novel Applications in Enzymatic Conversion of Carbon Dioxide

et al. 2017

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Turning carbon dioxide (CO 2 ) into fuels and chemicals using chemical, photochemical, electrochemical, and enzymatic methods could be used to recycle large quantities of carbon. The enzymatic method, which is inspired by cellular CO 2 metabolism, has attracted considerable attention for efficient CO 2 conversion due to improved selectivity and yields under mild reaction conditions. In this review, the research progress of green and potent enzymatic conversion of CO 2 into useful fuels and chemicals was discussed. Furthermore, applications of the enzymatic conversion of CO 2 to assist in CO 2 capture and sequestration were highlighted. A summary including the industrial applications, barriers, and some perspectives on the research and development of the enzymatic approach to convert CO 2 were introduced.

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“…[ 8,15 ] To make sure that in this biocatalyzed system, incorporated with photochemical NADH regeneration, the methanol actually did originate from CO 2 rather than from any other carbon residues in the reaction mixture, a set of control experiments in the absence of CO 2 was performed. These control experiments failed to produce any detectable methanol, which clearly confi rmed the origin of methanol from CO 2 .…”

Section: Integrated Artifi Cial Photosynthesis For Methanol Synthesmentioning

confidence: 99%

“…[7] Recently, an integrated photocatalyst based on chemically converted graphene with a covalently attached isatin-porphyrin chromophore showed a high electron-transfer efficiency and excellent stability and reusability in the photo-regeneration of NADH. [8] Such integration, however, was only for the photocatalysis part, all other active components involved in the biocatalysis part were not really integrated. To realize real integration of the whole system, it remains a challenge to design a multicomponent system with a controlled structural arrangement.…”

mentioning

confidence: 99%

Integration of Artificial Photosynthesis System for Enhanced Electronic Energy‐Transfer Efficacy: A Case Study for Solar‐Energy Driven Bioconversion of Carbon Dioxide to Methanol

Wang

et al. 2016

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Biocatalyzed artificial photosynthesis systems provide a promising strategy to store solar energy in a great variety of chemicals. However, the lack of direct interface between the light-capturing components and the oxidoreductase generally hinders the trafficking of the chemicals and photo-excited electrons into the active center of the redox biocatalysts. To address this problem, a completely integrated artificial photosynthesis system for enhanced electronic energy-transfer efficacy is reported by combining co-axial electrospinning/electrospray and layer-by-layer (LbL) self-assembly. The biocatalysis part including multiple oxidoreductases and coenzymes NAD(H) was in situ encapsulated inside the lumen polyelectrolyte-doped hollow nanofibers or microcapsules fabricated via co-axial electrospinning/electrospray; while the precise and spatial arrangement of the photocatalysis part, including electron mediator and photosensitizer for photo-regeneration of the coenzyme, was achieved by ion-exchange interaction-driven LbL self-assembly. The feasibility and advantages of this integrated artificial photosynthesis system is fully demonstrated by the catalyzed cascade reduction of CO2 to methanol by three dehydrogenases (formate, formaldehyde, and alcohol dehydrogenases), incorporating the photo-regeneration of NADH under visible-light irradiation. Compared to solution-based systems, the methanol yield increases from 35.6% to 90.6% using the integrated artificial photosynthesis. This work provides a novel platform for the efficient and sustained production of a broad range of chemicals and fuels from sunlight.

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Highly Selective Solar-Driven Methanol from CO₂ by a Photocatalyst/Biocatalyst Integrated System

Cited by 202 publications

References 34 publications

Face the Edges: Catalytic Active Sites of Nanomaterials

Face the Edges: Catalytic Active Sites of Nanomaterials

Recent Progress and Novel Applications in Enzymatic Conversion of Carbon Dioxide

Integration of Artificial Photosynthesis System for Enhanced Electronic Energy‐Transfer Efficacy: A Case Study for Solar‐Energy Driven Bioconversion of Carbon Dioxide to Methanol

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Highly Selective Solar-Driven Methanol from CO2 by a Photocatalyst/Biocatalyst Integrated System

Cited by 202 publications

References 34 publications

Face the Edges: Catalytic Active Sites of Nanomaterials

Face the Edges: Catalytic Active Sites of Nanomaterials

Recent Progress and Novel Applications in Enzymatic Conversion of Carbon Dioxide

Integration of Artificial Photosynthesis System for Enhanced Electronic Energy‐Transfer Efficacy: A Case Study for Solar‐Energy Driven Bioconversion of Carbon Dioxide to Methanol

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Highly Selective Solar-Driven Methanol from CO₂ by a Photocatalyst/Biocatalyst Integrated System