ACS Applied Materials & Interfaces
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2022
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IF 10.383
Xiewen Wu,Song Wang,Jing Fang,Hui Chen,Hongbo Liu,Run Li
Inspired by natural photosynthesis, photocatalytic NADH regeneration has drawn increasing interest in the recent decade as it provides a perfect approach for NAD+ reduction into NADH, which can be further consumed by oxidordeuctase for enzymatic redox reactions. However, two issues still remain unsolved in this procedure. First, the photocatalytic efficiency in NAD+ hydrogenation requires further improvement. Second, the rhodium electron mediator [Cp*Rh(bpy)H2O]2+ (M), which is always required for selective 1,4-NADH regeneration, is difficult to recover because of its good solubility in aqueous solution. Given the high price of M, it is highly wasteful and inefficient if it only spends once. Here, we report a Cp*Rh(bpy)Cl implanted conjugated microporous polymer DTS/Rh@CMPs which can be employed as a highly effective visible light photocatalysts for in situ NADH regeneration without using additional M. In addition, the insertion of Rh complex into a polymer skeleton, as demonstrated in UV–vis, fluorescence, photocurrent and electrochemical impedance, dramatically improves the light absorption capacity and the electron separation and transfer efficiency. Compared with that of DTS@CMP-1 with M, an enhanced reaction yield of 33% was determined in DTS/Rh@CMP-1 suggesting that intramolecular electron transfer has a better activity than that of intermolecular electron transfer in photocatalytic NAD+ reduction. Moreover, as the Rh complex is rooted firmly in a polymer framework, negligible Rh loss and conversion decrease in NADH regeneration are observed. When the DTS/Rh@CMP-1 was coupled with yeast alcohol dehydrogenase (YADH, from Saccharomyces cerevisiae), 1.36 mM of methanol was accumulated, implying an excellent biocompatibility of DTS/Rh@CMP-1 and a high feasibility of photobiocatalysis for formaldehyde hydrogenation.
研究领域:
生物化学
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材料科学
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酶工程
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DOI
PubMed
高影响因子
ACS Catalysis
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2025
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IF 13.1
Shihao Li,Jiafu Shi,Yu Chen,Xinyu Mao,Shusong Liu,Yang Yang,Hong Wu,Zhongyi Jiang
Amino alcohols are widely used in chemical and pharmaceutical industries, while conventional synthesis methods face drawbacks such as low selectivity and high energy consumption. Multienzyme catalysis combined with light-driven cofactor regeneration affords a platform of light-driven synthesis of chemicals, where the transfer of electrons and protons as well as the route of enzymatic reactions dominates the energy conversion efficiency and atomic economy of carbon utilization. Herein, we construct a light-driven synthesis system comprising an energy-supplying module and a multienzyme catalytic module for 2-aminoethanol synthesis from formaldehyde and ammonia. First, a S-scheme heterojunction photocatalysts with a metal–organic framework core and a bipyridine-based conjugated polymer shell are prepared as an energy-supplying module. Through synergistic intensification of proton transfer and electron transfer, the photocatalysts render cofactor (NADH) regeneration efficiency with a turnover frequency of 30.49 h–1. Second, a multienzyme catalytic module is constructed for 2-aminoethanol synthesis in the presence of NADH. Under optimal conditions, this module produces 2-aminoethanol with an average reaction rate of 76.34 μmol L–1 h–1 within 24 h. Finally, the energy-supplying module is coupled with the multienzyme catalytic module for continuous synthesis of 2-aminoethanol from formaldehyde and ammonia, generating 0.55 mmol L–1 2-aminoethanol after 4 light–dark cycles. In addition, triethanolamine (TEOA) and glucose, a biomass-derived carbon source, are both confirmed as effective electron donors for NADH regeneration and light-driven synthesis system. This work opens a pathway for the synthesis of amino alcohols and demonstrates a paradigm for the intensification of reaction processes.
研究领域:
生物化学
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绿色化学
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DOI
高影响因子
Inorganic Chemistry Frontiers
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2020
·Vol. 7
·期 13
·2434-2442
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IF 5.958
Changchao Jia,Wenjuan Hu,Yuanyuan Zhang,Chao Teng,Zupeng Chen,Jian Liu
The development of a metal-free photoelectrode film is of great significance. Herein, graphitic carbon nitride (g-C3N4) nanosheets with a concentration of up to 36 mg mL−1 were first obtained on a large scale using a wet ball-milling method. The obtained g-C3N4 nanosheets exhibit 6- and 8-times higher activity in terms of photocatalytic H2 evolution and nicotinamide adenine dinucleotide (NADH) regeneration than bulk g-C3N4, respectively. Furthermore, a uniform g-C3N4 film electrode was fabricated via the interfacial self-assembly of nanosheets at the air/water interface, which can be transferred onto various substrates. By coupling with graphene nanosheets, a g-C3N4/graphene hybrid film electrode was assembled at the interface, showing improved photoelectrochemical coenzyme NADH regeneration efficiency. The photoelectrochemical system uses water as the electron donor, which avoids the drawback of using additional sacrificial agents. This work presents a novel and facile method to prepare high-quality g-C3N4 hybrid films, and also provides a sustainable route for renewable energy conversion and biocatalytic applications.
研究领域:
材料科学
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生物化学
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可再生能源
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2017
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IF 2.843
Dong Yang,Hongjian Zou,Yizhou Wu,Jiafu Shi,Shaohua Zhang,Xiaodong Wang,Pingping Han,Zhenwei Tong,Zhongyi Jiang
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., photosystem I and photosystem II) and electron transport chains (ETCs), and utilize 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.
研究领域:
材料科学
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生物化学
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光催化
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DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
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2022
·Vol. 28
·期 55
·e202201430
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IF 5.02
Yuanyuan Zhang,Jian Liu
Graphical An artificial photosystem was constructed through the covalent attachment of Rh complex onto PCN. The integrated photocatalyst could regenerate NADH efficiently by integrating the light harvesting unit and the electron transfer unit through conjugated connection. By further coupling with FDH immobilized on the hydrophobic membrane, an enhanced HCOOH production could be obtained. Natural photosynthesis is a highly unified biocatalytic system, which coupled cofactor (NAD(P)H) regeneration and enzymatic CO 2 reduction efficiently for solar energy conversion. Mimicking nature, a novel system with Rh complex covalently grafted onto NH 2 -functionalized polymeric carbon nitride (NH 2 -PCN) was constructed. The integrated connection of the light-harvesting and electron mediation modules as Rh m3 -N-PCN could promote the efficient NAD + reduction to NADH. As a result, the integrated system exhibited a conversion of ∼66 % within 20 minutes. By further coupling in situ generated NADH with formate dehydrogenase (FDH), a photoenzymatic production of formic acid (HCOOH) from CO 2 was accomplished. Moreover, by immobilizing FDH onto a hydrophobic membrane, an enhanced HCOOH production of ∼5.0 mM can be obtained due to the concentrated CO 2 on the gas-liquid-solid three-phase interface. Our work herein provides an integrated strategy for coupling the anchored electron mediator with immobilized enzyme for enhanced artificial photosynthesis.
研究领域:
生物化学
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环境科学
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材料科学
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DOI
PubMed
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
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2025
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IF 3.7
Xinyu Chen,Jiahui Xie,Hui Wang,Yujie Tang,Yezhou Yang,Pilang Zheng,Qihua Yang,Xin Liu,Xiaobo Li
Graphical A novel composite material integrating β-ketoenamine-linked nano TPTTA COFs and a rhodium complex electron mediator into a mesoporous silica matrix is reported for photocatalytic NADH regeneration. This design enhances electron transfer, achieving a 75.7% NADH yield, 89.8% selectivity, and an initial rate of 8.7 g NADH •g Cat −1 •h −1 , with stable performance over four cycles. The photocatalytic regeneration of NADH represents an effective means of mimicking photosynthesis, but confronts the challenges of the charge separation, electron transfer, and the selectivity control in the surface reduction stage. Herein, we report a multifunctional composite material that embeds β-ketoenamine-linked nano TPTTA covalent organic frameworks (COFs) and electron mediator (rhodium complex, [Cp*Rh(bpy) (H 2 O)Cl 2 ] into a functional mesoporous silica matrix for photocatalytic NADH regeneration. This strategy enables the facilitation of the electron transfer process while maintaining the intrinsic properties of the COFs, providing flexibility in COFs design. The strategic integration of electron mediator and the shortened charge migration path due to the nanosized COFs results in an NADH regeneration yield of 75.7% and a selectivity of 89.8% for 1,4-NADH. The initial reaction rate for NADH regeneration attained 8.7 g NADH •g Cat −1 •h −1 , and the system showed no decrease in activity after four reaction cycles.
研究领域:
生物化学
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材料科学
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DOI
PubMed
高影响因子
GREEN CHEMISTRY
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2025
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IF 9.2
yang Zhou,LingLong Huang,Yuan Tao,ChangQing Luo,Jian-Miao Xu,Zhi-Qiang Liu,Yu-Guo Zheng
The efficient regeneration of nicotinamide adenine dinucleotide (NADH), a key coenzyme in biocatalytic redox reactions, is essential for achieving sustainable chemical synthesis. However, existing 1,4-NADH regeneration methods generally suffer from high cost and poor stability, which limit their potential for industrial-scale applications.We proposed an innovative green electrochemical catalytic system for efficient regeneration of 1,4-NADH, which achieving a coenzyme conversion rate exceeding 99.0% through optimization of electrode materials and reaction conditions. In this study, cyclic voltammetry was used to investigate the effective potentials of multiple metal electrodes in the NAD+ reduction process, and the key factors affecting the NAD+ reduction efficiency were deeply resolved, revealing the complex mechanisms of the role of different electrode materials in the electron transfer and protonation processes. It was found that the introduction of foam metal and carbon nanoparticles could significantly enhance the electron transfer efficiency and increase the conversion of 1,4-NADH to 99.3%. In addition, the metal-carbon composite electrode prepared by sintering technique further enhanced the electron transfer efficiency and excellent stability. This study provides a new idea for the recycling of 1,4-NADH and contributes important insights for the efficiency improvement of electrochemical catalytic systems. Through material innovation and reaction optimization, this study demonstrates the key pathways to achieve sustainable chemical processes and opens up new directions for green chemical synthesis. In addition, it has the potential to advance biocatalytic technology in industrial applications and shows promising applications in biocatalysis and energy conversion.
研究领域:
生物化学
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电化学
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可持续化学合成
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DOI
高影响因子
CURRENT MICROBIOLOGY
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2019
·Vol. 76
·期 6
·706-712
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IF 1.595
Li Minghua,Meng Xiumei,Sun Zhiyang,Zhu Chunjie,Ji Huiying
It is well known that cofactors play a key role in the production of different compounds in bioconversion processes, while the high cost of cofactors limits their usage in industrial applications. In the present study, a NADH regeneration system was successfully developed in Lactobacillus plantarum by expressing the fdh gene coding for formate dehydrogenase (FDH) from Candida boidinii. Results indicated that the FDH was expressed with the highest activity of 0.82 U/mg of protein when cells entered early stationary phase. In addition, the expression of FDH increased the intracellular level of NADH and NADH/NAD + ratio in L. plantarum , and therefore, enhanced the NADH-dependent production of 3-phenyllactic acid (PLA) in repeated and fed-batch bioconversions. In brief, the results demonstrate that the NADH regeneration by expressing FDH is a promising strategy for producing NADH-dependent microbial metabolites in L. plantarum .
研究领域:
微生物学
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生物技术
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代谢工程
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DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Chun-Hui Gao,Shi-Ming Zhang,Fang-Fang Feng,San-San Hu,Qian-Fan Zhao,Yong-Zheng Chen
Visible-light-driven nicotinamide adenine dinucleotide (NADH) regeneration is one of the most effective measures, and cadmium sulfide (CdS) materials are typically used as low-cost photocatalysts. The CdS photocatalysts, however, still suffer from low regeneration efficiency and poor cycle stability. In this work, the CdS quantum dots (QDs) less than 10 nm embedded onto silica gel (CdS QDs/Silica gel) were constructed for visible-light-driven NADH regeneration by a successive ionic layer adsorption reaction and ball milling method. Results demonstrate that the photosensitivity of the CdS QDs/Silica gel composite was 31 times higher than that of the bulk CdS. Moreover, the conduction band (CB) edge of the CdS QDs/Silica gel composite is −1.34 eV, which is more negative 0.5 eV than that of the bulk CdS. The obtained CdS QDs/Silica gel composites showed the highest NADH regeneration yields of 68.8% under visible-light (LED, 420 nm) illumination and can be reused for over 40 cycles. Finally, the bioactivity of NADH toward enzyme catalysis is further confirmed by the hydrogenation of benzaldehyde to benzyl alcohol catalyzed with an alcohol dehydrogenase as enzyme catalysis.
研究领域:
生物化学
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材料科学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Lihang Yan,Guanhua Liu,Jianqiao Liu,Jing Bai,Yaoxuan Li,Huaxun Chen,Liya Zhou,Jing Gao,Yanjun Jiang
The utilization of CO 2 has become an important issue aiming to the achievement of carbon neutrality. The enzyme electrocatalytic CO 2 reduction to produce carbonaceous fuels has been increasingly appealing. While the low CO 2 aqueous solubility severely limits the CO 2 reduction efficiency, and the expensive cofactor restricts the application potential. In this study, microporous UiO-66-NH 2 was firstly converted into hierarchically porous structure (HP-UiO-66-NH 2 ) containing both micropores and mesopores to simultaneously enhance the enrichment of CO 2 and the immobilization of formate dehydrogenase by optimizing the pore structure. The relative contents of the protein secondary structures were similar after immobilization. The mechanism of enzyme electrocatalytic CO 2 reduction was proposed. The enzyme stability was highly enhanced after immobilization and the CO 2 reduction was enhanced by the enzyme electrocatalytic system through the combination of CO 2 enrichment and electrocatalytic NADH regeneration. The optimized catalytic system can obtain formate yield of 1.826 mM in 3 h (5.57 times higher than the free enzyme system) with a generation rate of 6086.7 μmol g cat ‑1 h ‑1 .
研究领域:
生物化学
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环境科学
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材料科学
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DOI
高影响因子
Small
·
2023
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IF 13.3
Rui Pei,Jing Liu,Chuanyong Jing,Min Zhang
The reduction of carbon dioxide to valuable chemicals through enzymatic processes is regarded as a promising approach for the reduction of carbon dioxide emissions. In this study, an in vitro multi-enzyme cascade pathway is constructed for the conversion of CO 2 into dihydroxyacetone (DHA). This pathway, known as FFFP, comprises formate dehydrogenase (FDH), formaldehyde dehydrogenase (FaldDH), formolase (FLS), and phosphite dehydrogenase (PTDH), with PTDH serving as the critical catalyst for regenerating the coenzyme NADH. Subsequently, the immobilization of the FFFP pathway within the hydrogen-bonded organic framework (HOF-101) is accomplished in situ. A 1.8-fold increase in DHA yield is observed in FFFP@HOF-101 compared to the free FFFP pathway. This enhancement can be explained by the fact that within FFFP@HOF-101, enzymes are positioned sufficiently close to one another, leading to the elevation of the local concentration of intermediates and an improvement in mass transfer efficiency. Moreover, FFFP@HOF-101 displays a high degree of stability. In addition to the establishment of an effective DHA production method, innovative concepts for the tailored synthesis of fine compounds from CO 2 through the utilization of various multi-enzyme cascade developments are generated by this work.
研究领域:
生物化学
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环境科学
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材料科学
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DOI
PubMed
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2017
·Vol. 92
·期 9
·2477-2487
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IF 3.135
Niyomukiza Samuel,Teng Bao,Xian Zhang,Taowei Yang,Meijuan Xu,Xin Li,Irene Komera,Tuyishime Philibert,Zhiming Rao
BACKGROUND 2,3-Butanediol (2,3-BD) has a wide range of applications in chiral molecular synthesis, biofuel additives, and in food flavor additive manufacturing. Fermentation is a favorable method for 2,3-BD production. However, it requires much time and produces several NADH related byproducts which compete with 2,3-BD production. Bacillus subtilis has an excellent ability for 2,3-BD production by biocatalysis. However, its production is limited by low intracellular NADH and the reversible property of acetoin reductase (AR/2,3-BDH). The whole cell biocatalyst process with two different NADH regeneration systems was designed for efficient production of 2,3-BD in B. subtilis 168. RESULTS Formate dehydrogenase and glucose dehydrogenase for NADH regeneration were successfully co-expressed with acetoin reductase in B. subtilis 168. After optimization of biocatalyst bioconversion conditions, B. subtilis 168/pMA5- bdhA-Hpa II- fdh yielded 74.5 g L −1 of 2, 3-BD with 9.3 g L −1 h −1 productivity by fed batch and 115.4 g of 2,3-BD was achieved using same batch bacterium by three repeated batch bioconversions. On the other hand, 63.7 g L −1 of 2, 3-BD was produced with 7.92 g L −1 h −1 productivity by B. subtilis 168/pMA5- bdhA-Hpa II- gdh . To our knowledge, the volume productivity obtained here is the highest ever reported for biocatalysis. CONCLUSION A higher productivity of 2,3-BD from acetoin was achieved by whole cell biocatalysis with NADH regeneration systems in B. subtilis 168. This approach can be applied for NADH related bio-based chemicals production to improve titer, yield and productivity. © 2017 Society of Chemical Industry
研究领域:
生物化学
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微生物学
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代谢工程
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DOI
高影响因子
危险品化学品经营许可证（带存储）