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Intensifying Electron Utilization by Surface-Anchored Rh Complex for Enhanced Nicotinamide Cofactor Regeneration and Photoenzymatic CO_(2)Reduction

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Research 2021年第1期2021卷 507-517页

作者： Yuqing Cheng Jiafu Shi Yizhou Wu Xueying Wang Yiying Sun Ziyi Cai Yu Chen Zhongyi Jiang Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin University92 Weijin RoadNankai DistrictTianjin 300072China Collaborative Innovation Center of Chemical Science and Engineering(Tianjin) 92 Weijin RoadNankai DistrictTianjin 300072China School of Environmental Science&Engineering Tianjin University92 Weijin RoadNankai DistrictTianjin 300072China State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 10090China

Solar-driven photocatalytic regeneration of cofactors,including reduced nicotinamide adenine dinucleotide(NADH),reduced nicotinamide adenine dinucleotide phosphate(NADPH),and reduced flavin adenine dinucleotide(FADH_(2)),could ensure the sustainable energy supply of enzymatic reactions catalyzed by oxidoreductases for the efficient synthesis of ***,the elevation of cofactor regeneration efficiency is severely hindered by the inefficient utilization of electrons transferred on the surface of *** by the phenomenon of ferredoxin-NADP+reductase(FNR)anchoring on thylakoid membrane,herein,a homogeneous catalyst of rhodium(Rh)complex,[Cp_(∗)Rh(bpy)H_(2)O]^(2+),was anchored on polymeric carbon nitride(PCN)mediated by a tannic acid/polyethyleneimine(TA/PEI)adhesive layer,acquiring PCN@TA/PEI-Rh core@shell *** by visible light,electrons were excited from the PCN core,then transferred through the TA/PEI shell,and finally captured by the surface-anchored Rh for instant utilization during the regeneration of *** TA/PEI-Rh shell could facilitate the electron transfer from the PCN core and,more importantly,achieved~1.3-fold elevation of electron utilization efficiency compared with ***,the PCN@TA/PEI-Rh afforded the NADH regeneration efficiency of 37.8%after 20 min reaction under LED light(405 nm)illumination,over 1.5 times higher than PCN with free *** of the NADH regeneration system with formate dehydrogenase achieved continuous production of formate from carbon dioxide(CO_(2)).Our study may provide a generic and effective strategy to elevate the catalytic efficiency of a photocatalyst through intensifying the electron utilization.

关键词： enzymatic dinucleotide catalyst

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Efficient Conversion of Formaldehyde and Propanal to Methacrolein on Ionic Liquid-Functionalized Polymer Catalyst

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SSRN 2024年

作者： Bian, Yuhang Zheng, Xiaoyan Li, Jie Peng, Zhijian Wang, Gang Li, Chunshan School of Science China University of Geosciences Beijing100083 China State Key Laboratory of Mesoscience and Engineering CAS Key Laboratory of Green Process and Engineering Beijing Key Laboratory of Ionic Liquids Clean Process Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China School of Chemical Engineering University of Chinese Academy of Sciences Beijing100049 China Langfang Technological Center of Green Industry Langfang065801 China Longzihu New Energy Laboratory Zhengzhou Institute for Emerging Industrial Technology China

In recent years, the methacrolein (MAL) synthesis through the aldol condensation of formaldehyde (FA) with propanal (PA) has received great attention of researchers. Herein, an ionic liquid-functionalized polymer catalyst, which exhibited higher performance than common homogenous sec-amine catalyst, was developed for catalytic synthesis of MAL via aldol condensation of FA with PA. FT-IR, XPS, TG-DTA, and 13C MAS NMR were used to characterize the structural and physicochemical features. The influences of solvent and reaction conditions on the catalytic performance were also systematically studied and optimized. The in situ FT-IR spectroscopic experiments was performed to investigate the catalytic mechanism. Kinetic studies revealed that the activation energy of aldol condensation between the FA and PA was 51.6 kJ/mol. No obvious decay of catalytic performance was observed after twelve times cycle. © 2024, The Authors. All rights reserved.

关键词： Catalysis

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In-situ Construction of Sulfur-doped g-C_(3)N_(4)/defective g-C_(3)N_(4) Isotype Step-scheme Heterojunction for Boosting Photocatalytic H_(2) Evolution

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Chinese Journal of Structural Chemistry 2022年第1期41卷 25-33页

作者： Jing Zou Guodong Liao Jizhou Jiang Zhiguo Xiong Saishuai Bai Haitao Wang Pingxiu Wu Peng Zhang Xin Li School of Environmental Ecology and Biological Engineering School of Chemistry and Environmental EngineeringKey Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationWuhan Institute of TechnologyWuhan 430205China Key Laboratory of Rare Mineral Ministry of Natural ResourcesGeological Experimental Testing Center of Hubei ProvinceWuhan 430034China Semiconductor Electronic Special Gas of Hubei Engineering Research Center JingzhouHubei 434000China State Center for International Cooperation on Designer Low-Carbon&Environmental Materials(CDLCEM) School of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001China Institute of Biomass Engineering Key Laboratory of Energy Plants Resource and UtilizationMinistry of Agriculture and Rural AffairsSouth China Agricultural UniversityGuangzhou 510642China

The rational construction of a high-efficiency stepscheme heterojunctions is an effective strategy to accelerate the photocatalytic H_(2).Unfortunately,the variant energy-level matching between two different semiconductor confers limited the photocatalytic ***,a newfangled graphitic-carbon nitride(g-C_(3)N_(4))based isotype step-scheme heterojunction,which consists of sulfur-doped and defective active sites in one microstructural unit,is successfully developed by in-situ polymerizing N,N-dimethylformamide(DMF)and urea,accompanied by sulfur(S)***,the polymerization between the amino groups of DMF and the amide group of urea endows the formation of rich *** propulsive integration of S-dopants contributes to the excellent fluffiness and dispersibility of lamellar g-C_(3)N_(4).Moreover,the developed heterojunction exhibits a significantly enlarged surface area,thus leading to the more exposed catalytically active *** importantly,the simultaneous introduction of S-doping and defects in the units of g-C_(3)N_(4) also results in a significant improvement in the separation,transfer and recombination efficiency of photo-excited electron-hole ***,the resulting isotype step-scheme heterojunction possesses a superior photocatalytic H_(2) evolution activity in comparison with pristine g-C_(3)N_(4).The newly afforded metal-free isotype step-scheme heterojunction in this work will supply a new insight into coupling strategies of heteroatoms doping and defect engineering for various photocatalytic systems.

关键词： sulfur-doping defects isotype step-scheme heterojunction g-C_(3)N_(4) photocatalytic H_(2)

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A Comparative Study on the Thick Electrode Via Dry processing and Slurry Coating

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SSRN 2024年

作者： Liu, Haixiang Ren, Yufei Su, Chang Wu, Xiangkun Zhang, Lan College of Chemical Engineering Shenyang University of Chemical Technology Shenyang110142 China CAS Key Laboratory of Green Process and Engineering Beijing Key Laboratory of Ionic Liquids Clean Process State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China Langfang Green Industrial Technology Center Institute of Process Engineering Chinese Academy of Sciences Hebei065001 China Longzihu New Energy Laboratory Zhengzhou Institute of Emerging Industrial Technology Henan University Zhengzhou450000 China

The growing market of portable electronics and electric vehicles calls for lithium-ion batteries (LIBs) with higher energy density. Thick electrodes can reduce the mass ratio of inactive components and thus becoming a universal strategy to increase the energy density of LIBs. In this work, we prepare thick mesocarbon microbeads (MCMB) electrodes via both dry processing and slurry casting method. With low binder content of 2 wt.%, all electrodes show satisfying structure stability. It shows that the one-dimensional (1D) conductive agent (CA), vapor-grown carbon fiber (VGCF), can not only promote the electron transport within the electrode, but also guarantee the electrode integrity even when polytetrafluoroethylene (PTFE) was lithiated. Moreover, electrode with VGCF as CA can be obtained via the slurry casting method even with a high areal capacity of 6.76 mAh cm-2. Although the dry processing method could further increase the areal active material loading to a higher level, while lithiation of the binder, PTFE, seriously hindering its application. On the contrary, the slurry casting method with 1D CA may worth well for further study. © 2024, The Authors. All rights reserved.

关键词： Electrodes

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Assembly and Jamming of Polar Additive-Swollen Microgels at Liquid-Liquid Interfaces: From Inverse Pickering Emulsions to Hierarchical Functional Materials

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SSRN 2024年

作者： Ngai, To Guan, Xin Liu, Yang Xia, Yufei Tse, Ying-Lung Steve Department of Chemistry The Chinese University of Hong Kong Shatin Hong Kong College of Polymer Science and Engineering State Key Laboratory of Polymer Materials Engineering Sichuan University Chengdu610065 China State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China

HypothesisPoly-N-isopropylacrylamide (PNIPAM)-based microgels have attracted considerable attention as soft particulate stabilizers because of their deformability and functionality. However, the intrinsic hydrophilicity of microgel limits their applications in stabilizing water-in-oil (W/O) Pickering emulsions. Using various polar additives can improve the hydrophobicity of microgels, thus unlocking new possibilities in inverse Pickering emulsion formation and materials *** types of microgels were synthesized through free-radical precipitation polymerization with tailored physiochemical properties. The effect of various polar additives on the wettability, adsorption kinetics and interfacial behaviors of microgels were systematically investigated. Inverse W/O Pickering emulsions stabilized by additive-swollen microgels were utilized as template for the fabrication of functional materials with dual-stimuli responsiveness and hierarchical ***-swollen PNIPAM-based microgels exhibited enhanced hydrophobicity and superior emulsifying capability, which spontaneously assembled and jammed at oil-water interfaces, thereby significantly reducing the interfacial energy and forming a densely packed, elastic and responsive microgel monolayer. The feasibility of the strategy was verified for the formation of inverse W/O Pickering emulsions and high internal phase Pickering emulsions (HIPPEs). More importantly, this simple formation strategy of microgel-stabilized inverse W/O Pickering emulsions provided a new platform for the fabrication of functional materials with tunable inner structures from microscale (e.g., dual-stimuli core-shell microgels) to macroscale (e.g., hierarchical porous materials) that can be used for potential applications, such as recyclable contaminant removal and biosensing. © 2024, The Authors. All rights reserved.

关键词： Functional materials

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Construction of Active Cs and Zr Sites for Selective Production of Methyl Methacrylate on Cs/Zr/Sio2 Catalyst

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SSRN 2025年

作者： Yan, Tingting Deng, Senlin Wang, Gang Li, Jie Chang, Wei Zhang, Guoliang Li, Chunshan School of Chemical Engineering & Technology China University of Mining and Technology Jiangsu221116 China State Key Laboratory of Mesoscience and Engineering CAS Key Laboratory of Green Process and Engineering Beijing Key Laboratory of Solid-State Battery and Energy Storage Process Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China School of Chemical Engineering University of Chinese Academy of Sciences Beijing100049 China Longzihu New Energy Laboratory Henan University Zhengzhou450046 China Longzihu New Energy Laboratory Zhengzhou Institute of Emerging Industrial Technology Zhengzhou450046 China

Acid-base bifunctional Cs-Zr supported SiO2 exhibit high catalytic performance on aldol condensation of methyl propionate (MP) and formaldehyde (FA) toward methyl acrylate (MMA). However, the effect of structural configuration of surface active sites on the formation rate and selectivity of MMA remains unclear. In this study, a surface engineering strategy was proposed to directionally induce the formation of catalytically active centers. Comprehensive characterizations were performed to identify the structural configuration of surface active Cs and Zr sites and their influence on MMA production in combination with catalytic evaluation. It was discovered that the increased density of isolated hydroxyl groups (≡Si-OH) on SiO2 support after calcination treatment promoted the formation of well-defined Si-O-Zr and Si-O-Cs structures, corresponding to the medium strong acid and weak base sites. The acid-base properties and their balance of as-prepared Cs/Zr/SiO2 catalyst could be controllably modulated by the surface hydroxyl density and Cs (Zr) loading. These highly dispersed Cs and Zr species generated through the strong interaction with hydroxyl groups facilitated the production of MMA while suppressed the undesired MAL. Consequentially, the formation rate and selectivity of MMA could reach up to 0.91 mmol/h/gCat and 94.3% on the optimal 1.5Cs/0.25Zr/SiO2. Further mechanistic studies using in situ DRIFT revealed the catalytic pathway toward MMA and MAL, confirming the activation of MP was the kinetic-relevant step. © 2025, The Authors. All rights reserved.

关键词： Silicon compounds

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Kinetic and HPLC-MS analyses revealed the catalysis behavior of total saponins from MOF-based solid acids

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Journal of Molecular Liquids 2025年 429卷

作者： Zhang, YanXiao Gao, XiaoNing Xu, Juan Feng, Lu School of Chemistry and Environmental Engineering Key Laboratory of Green Chemical Engineering Process of Ministry of Education Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education State Key Laboratory of Green and Efficient Development of Phosphorus Resources Wuhan Institute of Technology Wuhan430073 China Hubei Key Laboratory of Processing and Application of Catalytic Materials Huanggang Normal University Huanggang438000 China Laboratory Department of Central Theater General Hospital of the Chinese People's Liberation Army Wuhan430000 China

Diosgenin is an influential intermediate for the preparation of various steroidal drugs, and has the reputation of "mother of hormones" and "medicinal gold". In this work, UiO-66-NH2 is quaternary ammoniated by functional modification of 3,5-diamino-1,2,4-triazole and then ion-exchanged with different concentrations of CF3SO3H to produce ionic liquids grafted MOF-based solid acids, namely UNS-0.96 and UNS-1.28, where 0.96 and 1.28 represent the volume (mL) of CF3SO3H consumed. They were used to extract diosgenin from total saponins, suggesting that UNS-1.28 can achieve high diosgenin extraction with a shorter time (2.5 h) and a lower addition amount (0.15 g) and the optimum diosgenin yield of 22.5 % was obtained. The extraction efficiency is higher than that obtained by hydrolysis of 2 M H2SO4 and commercial ion exchange resins. Kinetic studies have shown that the catalytic of total saponins by UNS-1.28 is in perfect agreement with the pseudo-first-order kinetic model, and that the activation energy required for extraction is low, only 2.83 × 104 J/mol. In addition, HPLC-MS was used to analyze the total saponins and products at different extraction times. The fragmentation peak types and relative abundances of the different extracted products are compared to reveal the cleavage pathways of the total saponins and the optimal period of diosgenin production, and to suggest the mechanism of action of the solid acid on the total saponins. © 2025 Elsevier B.V.

关键词： Kinetic parameters

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Self-assembling bile pigments for cancer diagnosis and therapy

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Aggregate 2021年第1期2卷 84-94页

作者： Kaiwei Chen Ruirui Xing Xuehai Yan State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijingChina School of Chemical Engineering University of Chinese Academy of SciencesBeijingChina Center for Mesoscience Institute of Process EngineeringChinese Academy of SciencesBeijingChina

Nanomaterials that integrate multiple functions provide promising opportunities for noninvasive and targeted cancer diagnosis and ***,the unclear metabolic pathway to nanomaterials brought difficulties to clinical *** bile pigments are endogenous functional materials with excellent biocompatibility and low *** materials based on endogenous bile pigments provide a decent solution to this *** this review,the features and functions of self-assembling bile pigments are discussed in detail for cancer diagnosis and treatment *** are put on the intrinsic physicochemical characteristics of bile pigments and their applications,including drug delivery,photoacoustic imaging,photothermal therapy,and anti-inflammation *** review will promote the exploration of these areas and tremendously realize the innovative applications of self-assembling biliverdin/bilirubin nanomaterials toward cancer diagnosis and therapy.

关键词： self-assembly endogenous bile pigments nanomaterials cancer diagnosis and therapy

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Systematic engineering of the sterol synthesis pathway for Saccharomyces cerevisiae promotes the efficient production of β-caryophyllene

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Metabolic engineering 2025年 91卷 347-355页

作者： Yapeng Zhang Chenwen Liu Wenqiang Li Zhidong Ma Bo Lv Lei Qin Chun Li Key Laboratory of Medical Molecule Science and Pharmaceutics Engineering Ministry of Industry and Information Technology/Institute of Biochemical Engineering School of Chemistry and Chemical Engineering Beijing Institute of Technology Beijing China Department of Chemical Engineering Tsinghua University Beijing China Key Lab for Industrial Biocatalysis Ministry of Education Tsinghua University Beijing China Center for Synthetic and Systems Biology Tsinghua University Beijing China Beijing Key Laboratory of Recombinant Protein Synthetic Biomanufacturing Beijing China State Key Laboratory of Green Biomanufacturing Beijing China

β-caryophyllene, a plant-derived sesquiterpene, serves as a food flavoring, anti-inflammatory agent, antioxidant, and high-energy fuel source. Extraction of β-caryophyllene from plants is a costly and inefficient process. Therefore, microbial cell factories have been employed for the production of β-caryophyllene. However, the limited yield is insufficient for its industrial application. In this study, we balanced the utilization of cellular resources for growth and production by systematically regulating the sterol synthesis pathway to maximize the synthesis of β-caryophyllene. In the competitive pathways concerning sterol and fatty acid synthesis, genes expression was suppressed by substituting the original promoters with a glucose-sensing promoter P HXT1 and a sterol synthesis promoter P ERG7 , respectively. This approach effectively increased the production of β-caryophyllene by 6.8 times, reaching 854.7 mg/L. engineering glucose-sensing pathway altered the strength of P HXT1 , resulting in an increase in β-caryophyllene production to 1.25 g/L. The cell growth and β-caryophyllene production were further boosted through diploid fusion, resulting in 21.4 g/L β-caryophyllene in fed-batch fermentation. This represents the highest reported production of β-caryophyllene to date. This study provides a valuable reference for the production of sesquiterpenes in microbial cell factories.

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Mn_(x)Co_(3-x)O_(4)Microtubules with Enhanced Catalytic Activity Towards Toluene Combustion:Effects of Redox Property and Oxygen Species

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China Petroleum processing & Petrochemical Technology 2021年第4期23卷 7-17页

作者： Zhang Hanyu Hu Yue Zhang Xiaohan Sun Mengyao Liu Rui Qi Jian Jin Quan Key Laboratory of Automobile Materials(Ministry of Education) School of Materials Science and EngineeringJilin UniversityChangchun 130022 School of Chemical Engineering Dalian University of TechnologyPanjin 124221 College of Environmental and Safety Engineering Shenyang University of Chemical TechnologyShenyang 110142 State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190

The redox property and oxygen species play an important role in the catalytic oxidation of volatile organic compounds(VOCs).In this paper,a series of Mn_(x)Co_(3-x)O_(4)catalysts with tubular structure were synthesized and applied for the catalytic combustion of *** characterization technologies were employed to reveal the relationship between the catalytic performance of the Mn_(x)Co_(3-x)O_(4)catalysts and Mn *** results of XRD,SEM and N2 adsorption-desorption analyses showed that the Mn doping had significant effects on the structure and morphology of the Mn_(x)Co_(3-x)O_(4)*** H2-TPR,O2-TPD,and XPS results proved that the strong interaction between Co and Mn resulted in the enhanced Olatt mobility,the richer active oxygen species,and the enhanced redox property in comparison with the pure Co_(3)O_(4)sample,which were crucial to the improvement of the catalytic activity of Co-Mn *** best catalyst,Co5-Mn5 sample,exhibited a good and stable activity to catalytically oxidize toluene at low temperatures even in the presence of water vapor,indicating that it is a potential material to be used in the commercialization of catalytic abatement of toluene.

关键词： catalytic combustion cobalt oxides manganese doping,toluene

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