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Insights into spin polarization regulated exciton dissociation and charge separation of C_(3)N_(4)for efficient hydrogen evolution and simultaneous benzylamine oxidation

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Nano Research 2023年第7期16卷 8845-8852页

作者： Gen Li Xiaomei Sun Peng Chen Meiyang Song Tianxiang Zhao Fei Liu Shuang-Feng Yin Provincial Guizhou Key Laboratory of Green Chemical and Clean Energy Technology School of Chemistry and Chemical EngineeringGuizhou UniversityGuiyang 550025China College of Chemistry and Chemical Engineering Advanced Catalytic Engineering Research Center of the Ministry of EducationState Key Laboratory of Chemo/Biosensing and ChemometricsHunan UniversityChangsha 410082China

The employment of spin polarization under an external magnetic field holds great potential for the improvements of photocatalytic ***,owing to the huge difference in dielectric properties between ferromagnetic oxide and polymers,the photogenerated excitons with spin states are often limited to the ferromagnetic oxide wells,which leads to unsatisfactory *** this paper,a single-atom Co-doped C_(3)N_(4)photocatalyst is successfully synthesized for photocatalytic water splitting and simultaneous oxidation of *** a tiny external magnetic field(24.5 mT),the hydrogen production rate could reach at 3979.0μmol·g^(-1)·h^(-1),which is about 340 times that of C_(3)N_(4).Experimental results and theoretical calculations indicate that the interaction of Co d and N p orbital changes the symmetry center of C_(3)N_(4),resulting in an increase in dielectric constant and spin ***,magnetic fields further promote parallel electron spin,and the increased number of charges with the parallel spin-down state is likely to dissociate under the action of an external magnetic *** the other hand,the Co-N bond provides a huge built-in electric field and active site for strengthening the charge transfer and surface *** work not only deepens the understanding of spin polarization,but also enriches methods to accelerate electron-hole separation.

关键词： low magnetic field C_(3)N_(4) spin polarization photocatalytic hydrogen evolution benzylamine oxidation

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engineering Corynebacterium glutamicum for the efficient production of 3-hydroxypropionic acid from glucose via theβ-alanine pathway

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Synthetic and Systems Biotechnology 2024年第4期9卷 752-758页

作者： Xiaodi Wang Junyuan Hou Jieyao Cui Zhiwen Wang Tao Chen Frontier Science Center for Synthetic Biology and Key Laboratory of Systems Bioengineering of the Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China School of Chemical Engineering and Technology Tianjin UniversityTianjin300072China

3-Hydroxypropionic Acid(3-HP)is recognized as a high value-added chemical with a broad range of *** the various biosynthetic pathways for 3-HP production,theβ-alanine pathway is particularly noteworthy due to its capacity to generate 3-HP from glucose at a high theoretical *** this study,theβ-alanine biosynthesis pathway was introduced and optimized in Corynebacterium *** strategically regulating the supply of precursors,we successfully engineered a strain capable of efficiently synthesizing 3-HP through theβ-alanine pathway,utilizing glucose as the *** engineered strain CgP36 produced 47.54 g/L 3-HP at a yield of 0.295 g/g glucose during the fed-batch fermentation in a 5 L fermenter,thereby attaining the highest 3-HP titer obtained from glucose via theβ-alanine pathway.

关键词： 3-Hydroxypropionic acid β-Alanine pathway Corynebacterium glutamicum Metabolic engineering

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Study on flow characteristics and phase holdup in a slurry bubble column coupled with mild agitation Author links open overlay panel

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Particuology 2024年第8期91卷 226-234页

作者： Qingyuan An Jiantao Li Lei Zhang Nailiang Wang Pengfei Zhang Zhenghong Luo Chunxi Lu State Key Laboratory of High-Efficiency Coal Utilization and Green Chemical Engineering Ningxia UniversityYinchuan750021China State Key Laboratory of Heavy Oil Processing College of Chemical Engineering and EnvironmentChina University of Petroleum BeijingBeijing102249China Department of Chemical&Biological Engineering Monash UniversityVictoria3800Australia

A pilot-scale experimental setup was constructed to investigate the effect of mild agitation on the bubble characteristics and phase holdup in a slurry bubble *** agitation positively impacts the axial uniform distribution of solid holdup,though it shows insignificant influence on the radial *** homogenous regime,mild agitation promotes the coalescence of bubbles,and the effect becomes stronger with increasing agitator *** mild agitation contributes to a decrease in bubble size in heterogeneous flow *** agitation presents a significant effect on the gas holdup by adjusting the bubble size and bubble motion *** modification was introduced to predict the gas holdup considering the effects of mild agitation,a necessary consideration for applications requiring mild *** adapted model predicts gas holdup with a maximum error of 12.9%.

关键词： Slurry bubble column Mild agitation Phase holdup Bubble characteristics

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Selective hydrodeoxygenation of polyethylene terephthalate plastic wastes into 1;4-dimethylcyclohexane by Ir-ReO_(x)/SiO_(2)+HZSM-5 catalytic system

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Science China Chemistry 2025年第4期68卷 1563-1575页

作者： Nan Wang Jieyi Liu Junde Wei Sibao Liu Guozhu Liu Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and Technology Tianjin 300072China Engineering Research Center of Polymer Green Recycling of Ministry of Education Fujian Key Laboratory of Pollution Control&Resource ReuseCollege of Environmental and ResourcesFujian Normal UniversityFuzhou 350007China Haihe Lab of Sustainable Chemical Transformations Tianjin 300192China

In order to mitigate the environmental impact of polyethylene terephthalate(PET)plastic pollution and enhance waste resource utilization;we developed a novel Ir-ReO_(x)/SiO_(2)+HZSM-5 catalytic system for the hydrodeoxygenation(HDO)of PET plastic wastes into cycloalkanes;particularly 1;4-dimethylcyclohexane(DMCH).Under mild conditions(190℃;3 MPa H_(2))with a certain amount of water in cyclopentane solvent;the highest yield of DMCH reached 95.8%;contributing to an overall yield of cycloalkanes at 98.4%within a reaction time of 4 h from HDO of virgin *** HDO of PET into DMCH involved initial hydrogenation of PET aromatic ring;then depolymerized by direct hydrogenolysis of acyl C-O bond in the ester group and subsequent cascade HDO of alcoholic C-O bond to saturated ester and alcohol intermediates;and further HDO of these oxygenates converting into desired DMCH *** Ir-ReO_(x)/SiO_(2) catalyst exhibits fully reduced metallic Ir nanoparticles along with partially reduced ReO_(x) species that are highly dispersed on both SiO_(2) surface and Ir nanoparticle *** oxophilic nature of ReO_(x) species facilitates the activation of C-O bonds;the acidic HZSM-5 zeolite for the promotion of dehydration reaction;and the protic property of H_(2)O for the enhancement of hydrogenation PET contributed to highly HDO activity of this ***;the catalytic system is applicable for the HDO of diverse real-world PET plastic wastes including Coca-ColaTM bottles;green Sprite bottles and white and red discarded fiber cloths;generating DMCH with a yield of up to 95.9%and cycloalkanes with a yield of up to 99.5%.This innovative process presents a new avenue for efficient hydrodeoxygenation conversion of PET into easily separable DMCH which serves as a crucial building block for the production of terephthalic acid to realize the chemical recycling of PET plastic wastes towards a green circular economy.

关键词： plastic wastes PET hydrodeoxygenation cycloalkane Ir-ReO_(x)/SiO_(2)

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Constructing an efficient deep-blue TADF emitter by host-guest interactions towards solution-processed OLEDs with narrowband emission

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Science China Chemistry 2023年第3期66卷 826-836页

作者： Yanchao Xie Lei Hua Zhi Wang Yuerong Liu Shian Ying Yuchao Liu Zhongjie Ren Shouke Yan Department Key Laboratory of Rubber-Plastics Ministry of Education/Shandong Provincial Key Laboratory of Rubber-PlasticsSchool of Polymer Science and EngineeringQingdao University of Science&TechnologyQingdao 266042China State Key Laboratory of Chemical Resource Engineering College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China

High-efficiency thermally activated delayed fluorescence(TADF) emitters and corresponding well-designed solution-processed organic light emitting diodes(OLEDs) are presently attractive due to their potential for exploiting large-area flexible displays. In this context, we innovatively integrate 2,12-di-tert-butyl-5,9-dioxa-13b-boronaphtho [3,2,1] anthracene as the acceptor with 3,6-bis(3,6-di-tert-butylcarbazol-N-yl) carbazole as the donor to construct a rigid deep-blue emitter, TB-3t BuCz, which exhibits a narrow emission with full-width-at-half-maximum(FWHM) of 46 nm. TB-3t BuCz itself dispalys no TADF characteristics both in solution or in pure film states. However, the significant TADF behavior can be observed when TB-3t BuCz is doped with 2,6-DCzPPy host due to the formation of exciplex-like species in 2,6-DCzPPy/TB-3t BuCz system. It is also found that the discernible spin-flip of triplet excitons is feasible when the S1/T1states of the formed exciplex stay slightly lower than S1 and T1states of TB-3t BuCz for the other host/TB-3t BuCz systems. Eventually, thanks to the synergetic effect of rigid structure and favorable photophysical properties of TB-3t BuCz, the solution-processed OLEDs based on 2,6-DCzPPy/TB-3t BuCz as emitting layer has achieved the significantly improved external quantum efficiency(EQE) of 14.6% with suppressed efficiency *** CIE1931 coordinate of(0.158, 0.052) is typically in deep-blue region. Note that, this EQE value is among the highest echelon of solution-processed OLEDs with deep-blue emission by utilizing boron-containing TADF emitters.

关键词： thermally activated delayed fluorescence oxygen-bridged cyclized boron host-guest interactions solution-processed OLEDs narrowband deep-blue emission

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Mechanisms and Mitigation Strategies of Gas Generation in Sodium-Ion Batteries

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Nano-Micro Letters 2025年第8期17卷 17-48页

作者： Xingyan Li Xi Chen Meng Li Haoran Wei Xuming Yang Shenghua Ye Liewu Li Jing Chen Xiangzhong Ren Xiaoping Ouyang Jianhong Liu Xiangtong Meng Jieshan Qiu Biwei Xiao Qianling Zhang Jiangtao Hu Graphene Composite Research Center College of Chemistry and Environmental EngineeringShenzhen UniversityShenzhen 518060People’s Republic of China GRINM(Guangdong)Research Institute for Advanced Materials and Technology Foshan 528051GuangdongPeople’s Republic of China School of Materials Science and Engineering Xiangtan UniversityXiangtan 411105People’s Republic of China College of Chemical Engineering State Key Laboratory of Organic-Inorganic CompositesState Key Laboratory of Chemical Resource EngineeringBeijing University of Chemical TechnologyBeijing 100029People’s Republic of China

The transition to renewable energy sources has elevated the importance of SIBs(SIBs)as cost-effective alternatives to lithium-ion batteries(LIBs)for large-scale energy *** review examines the mechanisms of gas generation in SIBs,identifying sources from cathode materials,anode materials,and electrolytes,which pose safety risks like swelling,leakage,and *** such as CO_(2),H_(2),and O_(2) primarily arise from the instability of cathode materials,side reactions between electrode and electrolyte,and electrolyte decomposition under high temperatures or *** mitigation strategies,encompassing electrolyte design,buffer layer construction,and electrode material optimization,are deliberated ***,subsequent research endeavors should prioritize long-term high-precision gas detection to bolster the safety and performance of SIBs,thereby fortifying their commercial viability and furnishing dependable solutions for large-scale energy storage and electric vehicles.

关键词： Sodium-ion batteries Gas evolution mechanism Inhibition strategies of gas generation High-performance sodium-ion battery roadmap

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Bifunctional two-carbon reagent made from acetylene via 1,2-difunctionalization and its applications

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Science China Chemistry 2024年第3期67卷 936-944页

作者： Bo Yang Kangkui Li Yongdong Wang Shifa Zhu Key Laboratory of Functional Molecular Engineering of Guangdong Province School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China School of Chemistry and Chemical Engineering Zhejiang Sci-Tech UniversityHangzhou 310018China Singfar Laboratories Guangzhou 510670China

There are very limited approaches to directly gluing two molecules for the production of internal alkenes using the vastly abundant acetylene via 1,2-difunctionalization. Conversion of gaseous acetylene to internal alkenes via 1,2-difunctionalization in a desired manner is not as easy as it might be expected due to the potential competition reactions between acetylene and alkene produced and the difficulty in handling this harmful reagent and controlling the regio-and stereoselectivity. In this work, we designed an efficient catalytic system for the incorporation of acetylene gas into tremendous(E)-β-bromo vinylsulfones, which are bench-stable, easy to operate, and can function as bifunctional acetylene and show a rich reactivity profile in Sonogashira coupling, Heck coupling, substituted reaction, and various desulfonylation transformations, providing numerous internal alkenes.

关键词： acetylene 1 2-difunctionalization photocatalysis vinylsulfone

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Manipulating micro-electric field and coordination-saturated site configuration boosted activity and safety of frustrated single-atom Cu/O Lewis pair for acetylene hydrochlorination

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Nano Research 2023年第7期16卷 9039-9049页

作者： Junchen Peng Dandan Dong Zongyuan Wang Hong Yang Dongyang Qiao Qinqin Wang Wei Sun Minmin Liu Jiajun Wang Mingyuan Zhu Bin Dai Fei He Chaofeng Huang School of Chemistry and Chemical Engineering/State Key Laboratory Incubation Base for Green Processing of Chemical Engineering Shihezi UniversityShihezi 832000China School of Chemistry and Chemical Engineering Southeast UniversityNanjing 211189China School of Materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of EducationTianjin UniversityTianjin 300072China College of Chemistry&Chemical Engineering Yantai UniversityYantai 264010China School of Material Science and Engineering University of JinanJinan 250022China

Simultaneously boosting acetylene hydrochlorination activity and avoiding formation of explosive copper acetylide over Cu-based catalyst,which represented a promising alternative to Hg-based and noble metal catalysts,remained ***,we fabricated a frustrated single-atom Cu/O Lewis pair catalyst(Cu/O-FLP)by coupling epoxide group(C-O-C)with atomdispersed Cu-cis-N_(2)C_(2)Cl center to address this *** basic epoxy site modulated the electron-deficient state of Lewisacidic Cu center and paired with the Cu-cis-N_(2)C_(2)Cl moiety to preferentially break HCl into different electronegative Cu-Clδ-and C-O-H^(δ+)intermediates,which further induced both an extra localized electric field to polarize acetylene and a upshift of the dband center of catalyst,thereby promoting adsorption and enrichment of acetylene by enhancing the dipolar interaction between acetylene and active ***,the generated Cu-Clδ-and C-O-H^(δ+)drastically reduced the energy barrier of ratelimiting step and made vinyl chloride easier to desorb from the Lewis-basic oxygen-atom site rather than traditional Lewis-acidic Cu *** superiorities ensured a higher activity of Cu/O-FLP compared with its ***,preferential dissociation of HCl endowed single-atom Cu with the coordination-saturated configuration,which impeded formation of explosive copper acetylide by avoiding the direct interaction between Cu and acetylene,ensuring the intrinsic safety during catalysis.

关键词： acetylene hydrochlorination Lewis pair single-atom Cu site configuration electric field

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Theoretically predicted innovative palladium stripe dopingcobalt(111) surface with excellent catalytic performance for carbonmonoxide oxidative coupling to dimethyl oxalate

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Chinese Journal of chemical engineering 2024年第9期73卷 235-243页

作者： Bingying Han Neng Shi Mengjie Dong Ye Liu Runping Ye Lixia Ling Riguang Zhang Baojun Wang State Key Laboratory of Clean and Efficient Coal Utilization Taiyuan University of TechnologyTaiyuan 030024China College of Chemical Engineering and Technology Taiyuan University of TechnologyTaiyuan 030024China College of Chemistry and Chemical Engineering Nanchang UniversityNanchang 330031China Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering Taiyuan 030013China

Pd-based catalysts are extensively employed to catalyze CO oxidative coupling to generate DMO,while the expensive price and high usage of Pd hinder its massive application in industrial *** Pd-based catalysts with high efficiency and low Pd usage as well as expounding the catalytic mechanisms are significant for the *** this study,we theoretically predict that Pd stripe doping Co(111)surface exhibits excellent performance than pure Pd(111),Pd monolayer supporting on Co(111)and Pd single atom doping Co(111)surface,and clearly expound the catalytic mechanisms through the density functional theory(DFT)calculation and micro-reaction kinetic model *** is obtained that the favorable reaction pathway is COOCH_(3)-COOCH_(3)coupling pathway over these four catalysts,while the rate-controlling step is COOCH_(3)+CO+OCH_(3)→2COOCH_(3)on Pd stripe doping Co(111)surface,which is different from the case(2COOCH_(3)→DMO)on pure Pd(111),Pd monolayer supporting on Co(111)and Pd single atom doping Co(111)*** study can contribute a certain reference value for developing Pd-based catalysts with high efficiency and low Pd usage for CO oxidative coupling to DMO.

关键词： CO oxidative coupling to DMO Pd stripe doping Co(111)surface Catalytic mechanism DFT calculation Micro-reaction kinetic model analysis Catalytic performance

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Recent advances in Ni-based catalysts for the electrochemical oxidation of ethanol

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Journal of Energy Chemistry 2024年第11期98卷 588-614页

作者： Xing Tan Shiming Chen Dafeng Yan Ruixing Du Qitong Zhong Longfei Liao Zhenchen Tang Feng Zeng State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816JiangsuChina School of Intelligent Medicine China Medical UniversityShenyang 110122LiaoningChina College of Chemistry and Chemical Engineering Hubei UniversityWuhan 430062HubeiChina School of Materials Science and Engineering Harbin Institute of Technology(Shenzhen)Shenzhen 518055GuangdongChina

The electrochemical ethanol oxidation reaction(EOR) plays a crucial role in electrochemical hydrogen production and direct ethanol fuel cells, both vital for utilizing renewable energies. Ni-based catalysts are pivotal in enabling efficient EOR, leading to the formation of acetic acid/acetaldehyde or CO_(2). These can serve as alternative anodic oxidation reactions for oxygen evolution reaction(OER) in water electrolysis or the anodic reaction for direct ethanol fuel cells, respectively. This review explores recent advancements in EOR over Ni-based catalysts. It begins with an overview of EOR performance across various Ni-based catalysts, followed by an examination of the reaction chemistry, mechanism, and active *** review then delves into strategies for designing highly active Ni-based EOR catalysts. These strategies include promotion with transition metals, noble metals, nonmetals, and carbon materials, as well as creating amorphous structures, special morphologies, and single-atom catalysts. Additionally, it discusses the concept of self-supporting catalysts using three-dimensional porous substrates. Finally, the review highlights emerging methodologies that warrant further exploration, along with future directions for designing highly active and stable EOR catalysts.

关键词： Ethanol oxidation Nickel Water electrolysis Fuel cell

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