Constructing quantum dots@flake g-C3N4 isotype heterojunctions for enhanced visible-light-driven NADH regeneration and enzymatic hydrogenation

Dong Yang, Hongjian Zou, Yizhou Wu, Jiafu Shi, Shaohua Zhang, Xiaodong Wang, Pingping Han, Zhenwei Tong, Zhongyi Jiang

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Abstract

NAD(P)H is a critical cofactor (biological source of hydrogen) that participates in many enzymatic hydrogenations for energy conversion and storage with resultant oxidation to NAD(P)+. Due to its high cost, the regeneration of NAD(P)H is a critical and feasible way to ensure the sustainability of these enzymatic hydrogenations. Intrigued by the photoreaction process in thylakoid membrane, we explored a two-dimensional (2D) isotype heterojunction photocatalyst, termed as quantum dots@flake graphitic carbon nitride (QDs@Flake g-C3N4), for visible-light-driven NAD(P)H regeneration. The catalyst was synthesized by one-step calcination using cyanamide-treated cyanuric acid-melamine (CM) complex as starting material, where cyanamide plays dual roles: a) assisting the transformation of CM from bulky to stacked structure and further to flakes after calcination, and b) acting as raw material for the generation of QDs on the flakes. To replicate both the functional and structural properties of the natural photoreaction system, QDs@Flake g-C3N4 exploited the two types of g-C3N4 (i.e., QDs and flake) and a heterojunction interface to, respectively, mimic the functional components of light-harvesting systems (LHSs, i.e., PS I and PS II) and electron transport chains (ETCs), and utilized the flake structure as the analogue of 2D thylakoid membrane. Therefore, QDs@Flake g-C3N4 showed remarkably improved capability in visible light harvesting and charge separation, and exhibited elevated performance in photocatalytic NADH regeneration with a regeneration yield of up to 40%. The NADH regeneration approach was then coupled with alcohol dehydrogenase-catalyzed hydrogenation of formaldehyde, achieving continuous methanol production.
Original languageEnglish
Pages (from-to)6247–6255
Number of pages9
JournalIndustrial & Engineering Chemistry Research
Volume56
Issue number21
Early online date10 May 2017
DOIs
Publication statusPublished - 31 May 2017

Fingerprint

NAD
Semiconductor quantum dots
Hydrogenation
Heterojunctions
Melamine
Calcination
Cyanamide
Membranes
Hydrogen
Carbon nitride
Acids
Photocatalysts
Energy conversion
Formaldehyde
Energy storage
Structural properties
Sustainable development
Raw materials
Methanol
Alcohols

Keywords

  • NADH regeneration
  • enzymatic hydrogenation
  • isotype herterojunctions
  • quantum dots
  • flake g-C3N4

Cite this

Constructing quantum dots@flake g-C3N4 isotype heterojunctions for enhanced visible-light-driven NADH regeneration and enzymatic hydrogenation. / Yang, Dong; Zou, Hongjian; Wu, Yizhou; Shi, Jiafu ; Zhang, Shaohua; Wang, Xiaodong; Han, Pingping; Tong, Zhenwei; Jiang, Zhongyi.

In: Industrial & Engineering Chemistry Research, Vol. 56, No. 21, 31.05.2017, p. 6247–6255.

Research output: Contribution to journalArticle

Yang, Dong ; Zou, Hongjian ; Wu, Yizhou ; Shi, Jiafu ; Zhang, Shaohua ; Wang, Xiaodong ; Han, Pingping ; Tong, Zhenwei ; Jiang, Zhongyi. / Constructing quantum dots@flake g-C3N4 isotype heterojunctions for enhanced visible-light-driven NADH regeneration and enzymatic hydrogenation. In: Industrial & Engineering Chemistry Research. 2017 ; Vol. 56, No. 21. pp. 6247–6255.
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abstract = "NAD(P)H is a critical cofactor (biological source of hydrogen) that participates in many enzymatic hydrogenations for energy conversion and storage with resultant oxidation to NAD(P)+. Due to its high cost, the regeneration of NAD(P)H is a critical and feasible way to ensure the sustainability of these enzymatic hydrogenations. Intrigued by the photoreaction process in thylakoid membrane, we explored a two-dimensional (2D) isotype heterojunction photocatalyst, termed as quantum dots@flake graphitic carbon nitride (QDs@Flake g-C3N4), for visible-light-driven NAD(P)H regeneration. The catalyst was synthesized by one-step calcination using cyanamide-treated cyanuric acid-melamine (CM) complex as starting material, where cyanamide plays dual roles: a) assisting the transformation of CM from bulky to stacked structure and further to flakes after calcination, and b) acting as raw material for the generation of QDs on the flakes. To replicate both the functional and structural properties of the natural photoreaction system, QDs@Flake g-C3N4 exploited the two types of g-C3N4 (i.e., QDs and flake) and a heterojunction interface to, respectively, mimic the functional components of light-harvesting systems (LHSs, i.e., PS I and PS II) and electron transport chains (ETCs), and utilized the flake structure as the analogue of 2D thylakoid membrane. Therefore, QDs@Flake g-C3N4 showed remarkably improved capability in visible light harvesting and charge separation, and exhibited elevated performance in photocatalytic NADH regeneration with a regeneration yield of up to 40{\%}. The NADH regeneration approach was then coupled with alcohol dehydrogenase-catalyzed hydrogenation of formaldehyde, achieving continuous methanol production.",
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author = "Dong Yang and Hongjian Zou and Yizhou Wu and Jiafu Shi and Shaohua Zhang and Xiaodong Wang and Pingping Han and Zhenwei Tong and Zhongyi Jiang",
note = "The authors thank the financial support from National Natural Science Funds of China (21406163, 91534126, 21621004), Tianjin Research Program of Application Foundation and Advanced Technology (15JCQNJC10000), Open Funding Project of the National Key Laboratory of Biochemical Engineering (2015KF-03), and the Program of Introducing Talents of Discipline to Universities (B06006). X.W. also acknowledges financial support from The Carnegie Trust for the Universities of Scotland (70265) and The Royal Society (RG150001 and IE150611).",
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T1 - Constructing quantum dots@flake g-C3N4 isotype heterojunctions for enhanced visible-light-driven NADH regeneration and enzymatic hydrogenation

AU - Yang, Dong

AU - Zou, Hongjian

AU - Wu, Yizhou

AU - Shi, Jiafu

AU - Zhang, Shaohua

AU - Wang, Xiaodong

AU - Han, Pingping

AU - Tong, Zhenwei

AU - Jiang, Zhongyi

N1 - The authors thank the financial support from National Natural Science Funds of China (21406163, 91534126, 21621004), Tianjin Research Program of Application Foundation and Advanced Technology (15JCQNJC10000), Open Funding Project of the National Key Laboratory of Biochemical Engineering (2015KF-03), and the Program of Introducing Talents of Discipline to Universities (B06006). X.W. also acknowledges financial support from The Carnegie Trust for the Universities of Scotland (70265) and The Royal Society (RG150001 and IE150611).

PY - 2017/5/31

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N2 - NAD(P)H is a critical cofactor (biological source of hydrogen) that participates in many enzymatic hydrogenations for energy conversion and storage with resultant oxidation to NAD(P)+. Due to its high cost, the regeneration of NAD(P)H is a critical and feasible way to ensure the sustainability of these enzymatic hydrogenations. Intrigued by the photoreaction process in thylakoid membrane, we explored a two-dimensional (2D) isotype heterojunction photocatalyst, termed as quantum dots@flake graphitic carbon nitride (QDs@Flake g-C3N4), for visible-light-driven NAD(P)H regeneration. The catalyst was synthesized by one-step calcination using cyanamide-treated cyanuric acid-melamine (CM) complex as starting material, where cyanamide plays dual roles: a) assisting the transformation of CM from bulky to stacked structure and further to flakes after calcination, and b) acting as raw material for the generation of QDs on the flakes. To replicate both the functional and structural properties of the natural photoreaction system, QDs@Flake g-C3N4 exploited the two types of g-C3N4 (i.e., QDs and flake) and a heterojunction interface to, respectively, mimic the functional components of light-harvesting systems (LHSs, i.e., PS I and PS II) and electron transport chains (ETCs), and utilized the flake structure as the analogue of 2D thylakoid membrane. Therefore, QDs@Flake g-C3N4 showed remarkably improved capability in visible light harvesting and charge separation, and exhibited elevated performance in photocatalytic NADH regeneration with a regeneration yield of up to 40%. The NADH regeneration approach was then coupled with alcohol dehydrogenase-catalyzed hydrogenation of formaldehyde, achieving continuous methanol production.

AB - NAD(P)H is a critical cofactor (biological source of hydrogen) that participates in many enzymatic hydrogenations for energy conversion and storage with resultant oxidation to NAD(P)+. Due to its high cost, the regeneration of NAD(P)H is a critical and feasible way to ensure the sustainability of these enzymatic hydrogenations. Intrigued by the photoreaction process in thylakoid membrane, we explored a two-dimensional (2D) isotype heterojunction photocatalyst, termed as quantum dots@flake graphitic carbon nitride (QDs@Flake g-C3N4), for visible-light-driven NAD(P)H regeneration. The catalyst was synthesized by one-step calcination using cyanamide-treated cyanuric acid-melamine (CM) complex as starting material, where cyanamide plays dual roles: a) assisting the transformation of CM from bulky to stacked structure and further to flakes after calcination, and b) acting as raw material for the generation of QDs on the flakes. To replicate both the functional and structural properties of the natural photoreaction system, QDs@Flake g-C3N4 exploited the two types of g-C3N4 (i.e., QDs and flake) and a heterojunction interface to, respectively, mimic the functional components of light-harvesting systems (LHSs, i.e., PS I and PS II) and electron transport chains (ETCs), and utilized the flake structure as the analogue of 2D thylakoid membrane. Therefore, QDs@Flake g-C3N4 showed remarkably improved capability in visible light harvesting and charge separation, and exhibited elevated performance in photocatalytic NADH regeneration with a regeneration yield of up to 40%. The NADH regeneration approach was then coupled with alcohol dehydrogenase-catalyzed hydrogenation of formaldehyde, achieving continuous methanol production.

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KW - enzymatic hydrogenation

KW - isotype herterojunctions

KW - quantum dots

KW - flake g-C3N4

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JO - Industrial & Engineering Chemistry Research

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