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Molecular engineering binuclear copper catalysts for selective CO_(2) reduction to C_(2) products

Journal of Energy Chemistry 2024年第6期93卷 166-173,I0005页

作者： qi Zhao Kai Lei Bao Yu xia Rachel Crespo-Otero Devis Di Tommaso Department of Chemistry School of Physical and Chemical SciencesQueen Mary University of LondonLondonE14NSUK Key Laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service FailureState Key Laboratory of Materials Processing and Die&Mould TechnologySchool of Chemistry and Chemical EngineeringHuazhong University of Science and Technology(HUST)Wuhan 430074HubeiChina Department of Chemistry University College LondonLondonWC1H 0AJUK Digital Environment Research Institute Queen Mary University of LondonEmpire HouseLondon E11HHUK

Molecular copper catalysts serve as exemplary models for correlating the structure-reaction-mechanism relationship in the electrochemical CO_(2) reduction(eCO_(2)R),owing to their adaptable environments surrounding the copper metal *** investigation,employing density functional theory calculations,focuses on a novel family of binuclear Cu molecular *** modulation of their coordination configuration through the introduction of organic groups aims to assess their efficacy in converting CO_(2) to C_(2)*** findings highlight the crucial role of chemical valence state in shaping the characteristics of binuclear Cu catalysts,consequently influencing the eCO_(2)R behaviour,Notably,the Cu(Ⅱ)Cu(Ⅱ)macrocycle catalyst exhibits enhanced suppression of the hydrogen evolution reaction(HER),facilitating proton trans fer and the eCO_(2)R *** rthermore,we explo re the impact of diverse electro n-withdrawing and electron-donating groups coordinated to the macrocycle(R=-F,-H,and-OCH_3)on the electron distribution in the molecular *** placement of-OCH_3 groups in the macrocycles leads to a favourable oxidation state of the Cu centres and subsequent C-C coupling to form C_(2) *** research provides fundamental insights into the design and optimization of binuclear Cu molecular catalysts for the electrochemical conversion of CO_(2) to value-added C_(2) products.

关键词： Molecular catalyst design Selective CO_(2)reduction C_(2)products Density functional theory calculations

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Innovative mesenchymal stem cell treatments for fatty liver disease

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World Journal of Stem Cells 2024年第9期16卷 846-853页

作者： fei-qiong Gao Jia-qi Zhu Xu-Dong Feng Department of Endocrinology Affiliated Hangzhou First People’s HospitalSchool of MedicineWestlake UniversityHangzhou 310003Zhejiang ProvinceChina Laboratory Medicine Center Department of Clinical LaboratoryZhejiang Provincial People’s HospitalPeople’s Hospital of Hangzhou Medical CollegeHangzhou 310014Zhejiang ProvinceChina Department of Clinical Laboratory Ningbo Medical Center Lihuili HospitalAffiliated Lihuili Hospital of Ningbo UniversityNingbo 315000Zhejiang ProvinceChina

The incidence of non-alcoholic fatty liver disease(NAFLD)and alcohol-associated liver disease(ALD)is increasing year by year due to changes in the contemporary environment and dietary structure,and is an important public health problem *** is an urgent need to continuously improve the understanding of their disease mechanisms and develop novel therapeutic *** stem cells(MSCs)have shown promise as a potential therapeutic strategy in therapeutic studies of NAFLD and *** and ALD have different triggers and their specific mechanisms of disease progression are different,but both involve disease processes such as hepatocellular steatosis and potential fibrosis,cirrhosis,and even hepatocellular *** have metabolic regulatory,anti-apoptotic,antioxidant,and immunomodulatory effects that together promote liver injury repair and functional recovery,and have demonstrated positive results in preclinical *** editorial is a continuum of Jiang et al’s review focusing on the advantages and limitations of MSCs and their derivatives as therapeutics for NAFLD and *** detail how MSCs attenuate the progression of NAFLD by modulating molecular pathways involved in glucolipid metabolism,inflammation,oxidative stress,endoplasmic reticulum stress,and *** on recent advances,we discuss MSCs and their derivatives as therapeutic strategies for NAFLD and ALD,providing useful information for their clinical application.

关键词： Alcohol-associated liver disease Non-alcoholic fatty liver disease Mesenchymal stem cells Cell therapy Inflammation

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Programmable synthetic receptors:the next-generation of cell and gene therapies

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Signal Transduction and Targeted Therapy 2024年第2期9卷 376-400页

作者： fei Teng Tongtong Cui Li Zhou qingqin Gao qi Zhou Wei Li University of Chinese Academy of Sciences Beijing 101408China State Key Laboratory of Stem Cell and Regenerative Biology Institute of ZoologyChinese Academy of SciencesBeijing 100101China Institute for Stem Cell and Regeneration Chinese Academy of SciencesBeijing 100101China Beijing Institute for Stem Cell and Regenerative Medicine Beijing 100101China

Cell and gene therapies hold tremendous promise for treating a range of difficult-to-treat ***,concerns over the safety and efficacy require to be further addressed in order to realize their full *** receptors,a synthetic biology tool that can precisely control the function of therapeutic cells and genetic modules,have been rapidly developed and applied as a powerful *** designed and engineered,they can be applied to finetune the therapeutic activities,i.e.,to regulate production of dosed,bioactive payloads by sensing and processing user-defined signals or *** review provides an overview of diverse synthetic receptor systems being used to reprogram therapeutic cells and their wide applications in biomedical *** a special focus on four synthetic receptor systems at the forefront,including chimeric antigen receptors(CARs)and synthetic Notch(synNotch)receptors,we address the generalized strategies to design,construct and improve synthetic ***,we also highlight the expanding landscape of therapeutic applications of the synthetic receptor systems as well as current challenges in their clinical translation.

关键词： synthetic landscape payload

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Stepwise colloidal lithography toward scalable and various planar chiral metamaterials

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Rare Metals 2024年第2期43卷 723-735页

作者： Xiu Yang Yong Liu fei-Liang Chen qian-qi Lin Rohit Chikkaraddy Shan-Shan Huang Shi-Lin xian Yi-Dong Hou Jing-Lei Du Liang-Ping xia Chun-Lei Du School of Electronic Science and Engineering University of Electronic Science and Technology of ChinaChengdu610054China School of Optoelectronic Science and Engineering University of Electronic Science and Technology of ChinaChengdu610054China Zhuhai Multiscale Optoelectronics Technology Co. Ltd.Zhuhai915060China Hybrid Materials for Opto-Electronics Group Department of Molecules and MaterialsMESA+Institute for NanotechnologyMolecules Center and Center for Brain-Inspired Nano SystemsFaculty of Science and TechnologyUniversity of Twente7500 AEEnschedeThe Netherlands School of Physics and Astronomy University of BirminghamBirminghamB152TTUK College of Physics Sichuan UniversityChengdu610065China Key Laboratory of Micro Nano Optoelectronic Devices and Intelligent Perception Systems Yangtze Normal UniversityChongqing408100China

Chiral metamaterials(CMs)composed by artificial chiral resonators have attracted great attentions in the recent decades due to their strong chiroptical resonance and identifiable interaction with chiral materials,facilitating practical applications in chiral biosensing,chiral emission,and display ***,the complex geometry of CMs improves the fabrication difficulty and hinders their scalable fabrication for practical applications,especially in the visible and ultraviolet *** potential strategy is the colloidal lithography that enables parallel fabrication for scalable and various planar ***,we demonstrate a stepwise colloidal lithography technique that uses sequential deposition from multiple CMs and expand their variety and *** geometry and optical chirality of building blocks from single deposition are systematically investigated,and their combination enables a significant extension of the range of chiral patterns by multiple-step *** approach resulted in a myriad of complex designs with different characteristic sizes,compositions,and shapes,which are particularly beneficial for the development of nanophotonic *** addition,we designed a flexible chiral device based on PDMS,which exhibits a good CD value and excellent stability even after multiple inward and outward *** excellent compatibility to various substrates makes the planar CMs more flexible in practical applications in microfluidic biosensing.

关键词： Chiral metamaterials Colloidal lithography Nanophotonics Metasurfaces Plasmonics Nanofabrications Flexible devices

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Low-cost dopant-free fluoranthene-based branched hole transporting materials for efficient and stable n-i-p perovskite solar cells

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Chinese Chemical Letters 2024年第10期35卷 187-193页

作者： Xinyu Yu fei Wu xianglang Sun Linna Zhu Baoyu xia Zhong'an Li Key Laboratory for Material Chemistry of Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Material Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China Chongqing Key Laboratory for Advanced Materials and Technologies of Clean Energy Faculty of Materials&EnergySouthwest UniversityChongqing 400715China

It has been widely recognized that hole transporting materials(HTMs)play a key role in the rapid progress of perovskite solar cells(PVSCs).However,common organic HTMs such as spiro-OMe TAD not only suffer from high synthetic costs,but also usually require the additional chemical doping process to improve their hole transport ability,which unfortunately induces the terrible stability ***,it is urgent to develop low-cost dopant-free HTMs for efficient and stable *** this work,we have successfully developed a new class of efficient dopant-free fluoranthene-based HTMs(TPF1–5)with quite low lab synthetic costs by combining donor-acceptor and branched structure *** detailed structure-property study revealed that tuning the twisted arms at different substitution sites would regulate the intermolecular interactions and film-forming ability,thereby significantly affecting the performance of the *** applying these HTMs in conventional PVSCs,the dopant-free TPF1-based devices not only achieved the best efficiency of 21.76%,which is comparable to that of the doped spiro-OMeTAD control devices,but also showed much better operational stability,which maintained over 87%of the initial efficiency under maximum power point tracking after 1038 h.

关键词： Perovskite solar cells Holetransporting materials Dopant-free Fluoranthene Low-cost

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Anisotropic microtopography surface of chitosan scaffold regulating skin precursor-derived Schwann cells towards repair phenotype promotes neural regeneration

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Regenerative Biomaterials 2024年第3期3卷 68-81页

作者： Meng Cong xia Wu Lingjie Zhu Guohao Gu fei Ding Guicai Li Haiyan Shi Key Laboratory of Neuroregenration of jiangsu and Ministry of Education and Co-Innovation Center of Neuroregeneration Nantong UniversityNantong 226001China Department of Pathophysiology School of MedicineNantong UniversityNantong 226001China

For repairing peripheral nerve and spinal cord defects,biomaterial scaffoid-based cell-therapy was emerged as an effective strategy,requiring the positive response of seed cells to biomaterial substrate and environment *** work highlighted that the imposed surface properties of scaffold could provide important guidance cues to adhered cells for ***,the insufficiency of native Schwann cells and unclear cellular response mechanisms remained to be *** that,this study aimed to illuminate the micropatterned chitosan-film action on the rat skin precursor-derived Schwann cells(SKP-SCs).Chitosanfilm with different ridge/groove size was fabricated and applied for the SKP-SCs *** indicated that SKP-SCs cultured on 30μm size microgroove surface showed better oriented alignment *** SKP-sCs presented similar genic phenotype as repair Schwann cells,increasing expression of c-Jun,neural cell adhesion molecule,and neurotrophic receptor ***,SKP-SC-secretome was subjected to cytokine array GS67 assay,data indicated the regulation of paracrine phenotype,a panel of cytokines was verifed up-regulated at secreted level and gene expression level in induced *** up-regulated cytokines exhibit a series of promotive neural regeneration functions,including cell survival,cell migration,cell proliferation,angiogenesis,axon growth,and cellular organization *** bioinformatics ***,the effectively polarized SKP-SCs-sourced secretome,promoted the proliferation and migration capacity of the primarily cultured native rat Schwann cells,and augmented neurites growth of the cultured motoneurons,as well as boosted axonal regrowth of the axotomy-injured *** together,SKP-SCs obtained pro-neuroregeneration phenotype in adaptive response to the anisotropic topography surface of chitosan-film,displayed the oriented parallel growth,the transition towards repair Schwann cell genic phenot

关键词： anisotropic microtopography skin precursor-derived Schwann cells chitosan-flm neural regeneration phenotype regulation

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Theoretical and experimental investigations on single-atom catalysis:Pt_(1)/FeO_(x) for water-gas shift reaction

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Nano Research 2024年第9期17卷 8627-8637页

作者： Shan-fei Wang Yangyang Li Haiyan Wang Jin-xia Liang Chun Zhu Botao qiao School of Chemistry and Chemical Engineering Guizhou UniversityGuiyang 550025China CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing 100049China

Oxide-supported metal single-atom catalysts(SACs)have exhibited excellent catalytic performance for water-gas shift(WGS)***,we report the single-atom catalyst Pt1/FeOx exhibits excellent medium temperature catalytic performance for WGS reactions by the density functional theory(DFT)calculations and experimental *** calculations indicate that H_(2)O molecules are easily dissociated at oxygen vacancies,and the formed*OH and*O are adsorbed on Pt1 single atoms and the adjacent O atoms,*** studying four possible reaction mechanisms,it is found that the optimal WGS reaction pathway is proceeded along the carboxyl mechanism(pathway III),in which the formation of*COOH intermediates can promote the stability of Pt_(1)/FeO_(x) SAC and the easier occurrence of WGS *** energy barrier of the rate-determining step during the entire reaction cycle is only 1.16 eV,showing the high activity for the medium temperature WGS reaction on Pt_(1)/FeO_(x) SAC,which was verified by experimental ***,the calculated turnover frequencies(TOFs)of CO_(2)and H_(2)formation on Pt1/FeOx at 610 K(337℃)can reach up to 1.14×10^(-3)s^(-1)·site^(-1)through carboxyl *** this work,we further expand the application potential of Pt1/FeOx SAC in WGS reaction.

关键词： water-gas shift(WGS)reaction single-atom catalyst(SAC) density functional theory(DFT) thermocatalysis

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Highly anti-corrosive NiFe LDHs–NiFe alloy hybrid enables long-term stable alkaline seawater electrolysis

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Rare Metals 2024年第9期43卷 4321-4332页

作者： Jia-Hong Li Hao Chen Si-Hang You Gan-Xin Yang Peng Liu Meng-qi Gao Shu-Guang Chen fei-fei Zhang School of Materials Science and Engineering Changsha University of Science and TechnologyHunan 410114China Department of Materials Science and Engineering Faculty of EngineeringNational University of SingaporeSingapore 117576Singapore School of Materials Science and Engineering Jilin UniversityJilin 130022China

Owing to the significant potential of alkalin seawater electrolysis for converting surplus power into eco friendly hydrogen fuel,we developed bifunctional elec trodes that integrate low-crystalline NiFe LDHs and amorphous NiFe alloy on a Ni foam(NF)substrate to enhance this *** by the battery-like charac teristics of NiFe LDHs,an anti-corrosive and active oute layer of NiFe^(vac)OOH continuously forms over time in th hybrid on the anode for the oxygen evolution reaction(OER),effectively mitigating powder shedding caused by corrosion induced by multiple anions in *** while,the strong bond between the hybrid and the NF substrate maintains intact hybrid coatings to ensure a rel atively high overall conductivity of the electrodes,signif icantly reducing the negative effects of structura degradation during the OER and hydrogen evolution reaction(HER),as well as the accumulation of contami nants on the electrode *** long-term tests,thes bifunctionalhybridelectrodesmaintained stable performance,even at a high current density o500 mA·cm^(-2).The cell voltage increased by only 88 m V over 1000 h to 1.970 V during saline electrolysis and by103 mV over 500 h to 2.062 V during seawater electroly ***,this study provides valuable insights into efficient and stable seawater electrolysis using NiFe LDHs–NiFe alloy hybrids.

关键词： NiFe LDHs Bifunctional Corrosion Stability Seawater electrolysis

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Should we perform sigmoidoscopy for colorectal cancer screening in people under 45 years?

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World Journal of Gastrointestinal Oncology 2024年第4期16卷 1248-1255页

作者： Waiian Leong Jia-qi Guo Chun Ning fei-fei Luo Rui Jiao Dong-Ye Yang Division of Gastroenterology&Hepatology The University of Hong Kong-Shenzhen HospitalShenzhen 518053Guangdong ProvinceChina Department of Accident&Emergency The University of Hong Kong-Shenzhen HospitalShenzhen 518053Guangdong ProvinceChina Department of Anatomical Pathology The University of Hong Kong-Shenzhen HospitalShenzhen 518053Guangdong ProvinceChina Endoscopy Center The University of Hong Kong-Shenzhen HospitalShenzhen 518053Guangdong ProvinceChin

BACKGROUND The strategy for preventing colorectal cancer is screening by colonoscopy,which offers a direct way for detection and removal of adenomatous polyps(APs).American College of Gastroenterology guidelines recommend that people aged≥45 years should undergo colonoscopy;however,how to deal with people aged≤45 years is still *** To compare the prevalence of APs and high-grade neoplasia between the left and right colon in patients≤45 *** A retrospective observational study was conducted at a single tertiary III hospital in *** study included patients aged 18-45 years with undergoing initial colonoscopy dissection and pathological diagnosis AP or high-grade neoplasia between February 2014 and January *** number of APs in the entire colon while screening and post-polypectomy surveillance in following 1-3 years were *** A total of 3053 cases were *** prevalence of APs in the left and right colon was 55.0%and 41.6%,respectively(OR 1.7,95%CI 1.6-2.4;P3 polyps(14.1%;OR 0.3,95%CI 0.1-0.6;P<0.05).CONCLUSION This study suggests that flexible sigmoidoscopy would be an optimal approach for initial screening in people aged≤45 years and would be a more cost-effective and safe strategy.

关键词： Adenomatous polyps High-grade neoplasia Colonoscopy Flexible sigmoidoscopy

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Peracetic acid catalytic activation using Co3O4 nanocluster decorated graphitic carbon nitride for cefapirin degradation in water

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Science China Technological Sciences 2024年第10期67卷 3103-3115页

作者： YIN ShiMei GAO YiXuan CHEN Long LI Fan LIU xiaoNa qi fei LIU Wen Beijing Key Lab for Source Control Technology of Water Pollution College of Environmental Science and EngineeringBeijing Forestry University Key Laboratory of Water and Sediment Sciences (Ministry of Education) College of Environmental Sciences and EngineeringPeking University School of Environmental Science and Engineering Taiyuan University of Technology State Environmental Protection Key Laboratory of All Material Fluxes in River Ecosystems Peking University Beijing National Laboratory for Molecular Sciences Peking University

This study innovated cobalt-based catalytic nanocomposites（CCNs） for the heterogeneous activation of peracetic acid（PAA）,a green and efficient advanced oxidation process for removing antibiotics from *** Co3O4catalysts exhibit limited activity due to stable electronic *** overcome this,CCNs were synthesized using a one-step condensation method,incorporating a size control strategy that anchors Co3O4nanoclusters within 4-5 nm onto six-fold cavity of g-C3N4,simultaneously modifying the coordination environment of *** alteration significantly enhances the adsorption energy of PAA and catalytic activity compared to commercial *** improved performance of CCN2,in particular,is attributed to a shift in the cobalt d band center towards the Fermi level,facilitating electron delocalization and transfer,enhancing Co-O bonding,and accelerating PAA ***2's superior activity,with a cefapirin（CFP） degradation kinetic rate constant(k1=0.760 min-1)～11 times that of PAA direct oxidation(k1=0.070 min-1) and～5 times that of commercial Co3O4/PAA system(k1=0.164 min-1),is due to its ability to generate dominant reactive species for antibiotic degradation,including alkoxy radicals(CH3C（=O）OO·),high valence metal(CoⅣ（=O）2+),and singlet oxygen（1O2）,with the latter two being crucial for the degradation *** degradation of CFP involved three mechanisms,including direct oxidation by PAA,decarboxylation,and open-ring reactions at nitrogen *** research provides insights into developing high-activity catalysts for efficient PAA activation and antibiotic removal,leveraging the strategy of shifting the transition metal d band center.

关键词： peracetic acid Co3O4 nanocluster high valence metal singlet oxygen cefapirin

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