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Identification of the optimal doping position of hetero-atoms in chalcogen-doped Fe-n-C catalysts for oxygen reduction reaction

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Particuology 2024年第6期89卷 99-108页

作者： Weihao liu Huanhuan He Qingtao liu Xin Wan Jianglan Shui School of Materials Science and Engineering Beihang UniversityBeijing100191China School of Space and Environment Beihang UniversityBeijing102206China Tianmushan Laboratory Hangzhou310023China

The excellent oxygen reduction reaction(ORR)activity of Fe–n–C catalysts in acidic media makes them potential for low-cost proton exchange membrane fuel *** recent years,it has been shown that heteroatoms(B,O,S,P,Cl,F,etc.)can be used as electron-withdrawing groups to modulate the planar structure and electron distribution of the Fe–nx active sites to achieve simultaneous improvement of catalytic activity and ***,the optimal location of the heteroatoms remains ***,taking chalcogen heteroatoms(S and Se)as an example,we control the doping positions and investigate their effect on the ORR performance of the Fe–n–C *** first coordination shell of the iron single atom is identified as the optimal doping *** optimized catalysts Fe–n_(3)Se_(1)/nC and Fe–n_(3)Se_(1)/nC demonstrate improved activity and stability in both half cells and fuel *** work provides insights into the enhancement mechanism of heteroatom doping in single-atom catalysts.

关键词： Oxygen reduction reaction Fe-n-C catalysts Hetero-atom doping Doping position Enhancement mechanism

Unlocking high-efficiency oxygen evolution reaction through Co-n coordination engineering in Co@n-doped porous carbon core–shell nanoparticles

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nano Research 2024年第8期17卷 7068-7076页

作者： Shucheng liu Yu Shuai Xiaosi Qi Zhao Ding Yi liu College of Big Data and Information Engineering Guizhou UniversityGuiyang 550025China College of Physics Guizhou Province Key Laboratory for Photoelectrics Technology and ApplicationGuizhou UniversityGuiyang 550025China

Modulation of metal sites coordination can significantly refine the electronic architecture of catalysts,thereby improving their catalytic *** work successfully developed a core–shell Co@n-doped porous carbon(Co@nC)catalyst by pyrolyzing the COF/MOF(IISERP-COF3/ZIF-67)composite in an inert *** Co@nC catalyst exhibited impressive oxygen evolution reaction(OER)performance,with a small overpotential of 304 mV and a modest Tafel slope of 88.6 mV·dec^(−1) in a 1 M KOH,alongside remarkable stability,maintaining 98.5%of its activity over 13 *** role of IISERP-COF3 was pivotal in preventing Co atom aggregation during the ZIF-67 pyrolysis,which facilitated the creation of mesopores for enhanced mass transport and ***,it effectively modulated the Co-n coordination to fine-tune the electronic structure,thereby optimizing the catalyst's capacity for adsorption of intermediates and boosting its intrinsic *** functional theory(DFT)studies corroborate that the exceptional OER efficiency of Co@nC can be linked to the enhanced Co-n coordination,optimizing the localized electronic structure at the Co active *** study not only proposes an innovative approach for optimizing COF/MOF as effective electrocatalysts but also clears the path for the emergence of affordable,high-performance alternatives to precious metal-based catalysts,marking a significant advancement in sustainable energy technologies.

关键词： covalent organic framework(COF) metal-organic framework(MOF) core-shell structure catalysts oxygen evolution reaction

Using vitamin C to improve both performance and stability of n-type organic semiconductors

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Science China Materials 2024年第11期67卷 3755-3756页

作者： Sizhe liu Xingxin Shao Jun liu Key Laboratory of Polymer Physics and Chemistry Changchun Institute of Applied ChemistryChinese Academy of Sciences School of Applied Chemistry and Engineering University of Science and Technology of China

Organic semiconductors(OSCs) have the great advantages of flexibility, light weight, low-cost and large-area processing [1].After intensively studied for several decades, OSCs are now considered to be the most promising candidate materials for next-generation electronic circuits. n-type OSCs are the vital component for the basic electronic element, such as p-n junctions, light-emitting diodes and complementary circuits [2].

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Inclusion of CoTiO_(3) to ameliorate the re/dehydrogenation properties of the Mg–na–Al system

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Journal of Magnesium and Alloys 2024年第3期12卷 1215-1226页

作者： n.A.Ali n.Y.Yusnizam n.A.Sazelee Sami-ullah Rather Haizhen liu M.Ismail Energy Storage Research Group Faculty of Ocean Engineering TechnologyUniversiti Malaysia Terengganu21030 Kuala NerusTerengganuMalaysia Department of Chemical and Materials Engineering King Abdulaziz UniversityP.O.Box80204Jeddah 21589Saudi Arabia Guangxi novel Battery Materials Research Center of Engineering Technology School of Physical Science and TechnologyGuangxi UniversityNanning 530004China State Key Laboratory of Featured Metal Materials and Life-Cycle Safety for Composite Structures Nanning 530004China

For the first time,the MgH_(2)–naAlH_(4)(ratio 4:1)destabilized system with CoTiO_(3) addition has been *** CoTiO_(3)-doped MgH_(2)–naAlH_(4) sample begins to dehydrogenate at 130℃,which is declined by 40℃ compared to the undoped MgH_(2)–naAlH_(4).Moreover,the de/rehydrogenation kinetics characteristics of the CoTiO_(3)-doped MgH_(2)–naAlH_(4) were greatly *** the inclusion of CoTiO_(3),the MgH_(2)–naAlH_(4) composite absorbed 5.2 wt.%H_(2),higher than undoped MgH_(2)–naAlH_(4).In the context of dehydrogenation,the CoTiO_(3)-doped MgH_(2)–naAlH_(4) sample desorbed 2.6 wt.%H_(2),almost doubled compared to the amount of hydrogen desorbed from the undoped MgH_(2)–naAlH_(4) *** activation energy obtained by the Kissinger analysis for MgH_(2) decomposition was significantly lower by 35.9 kJ/mol than the undoped MgH_(2)–naAlH_(4) *** reaction mechanism demonstrated that new phases of MgCo and AlTi_(3) were generated in situ during the heating process and are likely to play a substantial catalytic function and be useful in ameliorating the de/rehydrogenation properties of the destabilized MgH_(2)–naAlH_(4) system with the inclusion of CoTiO_(3).

关键词： Destabilize system Magnesium hydride Sodium alanate Hydrogen storage Additive.

Modulation of charge in C_(9)n_(4) monolayer for a highcapacity hydrogen storage as a switchable strategy

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Frontiers of physics 2024年第4期19卷 47-55页

作者： Lin Ju Junxian liu Minghui Wang Shenbo Yang Shuli liu School of Physics and Electric Engineering Anyang Normal UniversityAnyang 455000China School of Mechanical Medical and Process EngineeringQueensland University of TechnologyBrisbane QLD 4001Australia Hongzhiwei Technology(Shanghai)Co.Ltd. 1599 Xinjinqiao RoadPudongShanghai 201206China

Developing advanced hydrogen storage materials with high capacity and efficient reversibility is a crucial aspect for utilizing hydrogen source as a promising alternate to fossil *** this paper,we have systematically investigated the hydrogen storage properties of neutral and negatively charged C_(9)n_(4) monolayer based on density functional theory(DFT).Our foundings indicate that injecting additional electrons into the adsorbent significantly boosts the adsorption capacity of C_(9)n_(4) monolayer to H2 *** gravimetric density of negatively charged C_(9)n_(4) monolayer can reach up to 10.80 wt% when fully covered with *** other hydrogen storage methods,the storage and release processes happen automatically upon introducing or removing extra ***,these operations can be easily adjusted through activating or deactivating the charging *** a result,the method is easily reversible and has tunable kinetics without requiring particular ***,C_(9)n_(4) is proved to be a suitable candidate for efficient electron injection/release due to its well electrical *** work can serve as a valuable guide in the quest for a novel category of materials for hydrogen storage with high capacity.

关键词： hydrogen storage C_(9)n_(4)monolayer charge modulation density functional theory

Open-vessel Synthesis of Poly-n-methoxyethylglycine

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Chemical Research in Chinese Universities 2024年第1期40卷 153-158页

作者： liu Guojan MA Ke CHEn Qi ZHAnG Donghui liu Runhui State Key Laboratory of Bioreactor Engineering East China University of Science and TechnologyShanghai200237P.R.China Key Laboratory for Ultrafine Materials of Ministry of Education Frontiers Science Center for Materiobiology and Dynamic ChemistryShanghai Frontiers Science Center of Optogenetic Techniques for Cell MetabolismResearch Center for Biomedical Materials of Ministry of EducationSchool of Materials Science and EngineeringEast China University of Science and TechnologyShanghai200237P.R.China School of Biotechnology East China University of Science and TechnologyShanghai200237P.R.China

Polypeptoids are widely used in biological applications owing to their diverse functions and proteolytic *** type of polypeptoids,poly-n-methoxyethylglycine(P-nmeg),has been found to possess remarkable hydrophilicity and notable properties in terms of protein,cell,and bacterial ***,the currently known synthesis methods of P-nmeg include solid-phase synthesis,which is time-consuming and difficult to scale up,and n-substituted n-carboxyanhydride(nnCA)ring-opening polymerization,whose monomers were difficult to *** this study,we used the chemical stable nmeg n-phenoxycarbonyl(nPC)as the monomer,which was obtained without the use of highly toxic reactants,such as phosgene or phosphorus halide,to synthesize P-nmeg under open-vessel *** adding BnnH_(2) as an initiator at 80℃,we can obtain controllable short chain length P-nmeg with narrow dispersity.

关键词： Open-vessel Polypeptoid synthesis Poly-n-methoxyethylglycine Stable monomer narrow dispersity

Dysregulated n6-methyladenosine modification in peripheral immune cells contributes to the pathogenesis of amyotrophic lateral sclerosis

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Frontiers of Medicine 2024年第2期18卷 285-302页

作者： Di He Xunzhe Yang Liyang liu Dongchao Shen Qing liu Mingsheng liu Xue Zhang Liying Cui Department of neurology Peking Union Medical College Hospital(PUMCH)Chinese Academy of Medical Sciences and Peking Union Medical CollegeBeijing100730China Medical Doctor Program Chinese Academy of Medical Science and Peking Union Medical CollegeBeijing100730China McKusick-Zhang Center for Genetic Medicine State Key Laboratory of Medical Molecular BiologyInstitute of Basic Medical Sciences Chinese Academy of Medical SciencesSchool of Basic MedicinePeking Union Medical CollegeBeijing100730China neuroscience Center Chinese Academy of Medical Sciences and Peking Union Medical CollegeBeijing100730China

Amyotrophic lateral sclerosis(ALS)is a progressive neurogenerative disorder with uncertain *** evidence implicates n6-methyladenosine(m6A)modification in ALS *** RnA immunoprecipitation sequencing(MeRIP-seq)and liquid chromatography–mass spectrometry were utilized for m6A profiling in peripheral immune cells and serum proteome analysis,respectively,in patients with ALS(n=16)and controls(n=6).The single-cell transcriptomic dataset(GSE174332)of primary motor cortex was further analyzed to illuminate the biological implications of differentially methylated genes and cell communication *** of peripheral immune cells revealed extensive RnA hypermethylation,highlighting candidate genes with differential m6A modification and expression,including C-X3-C motif chemokine receptor 1(CX3CR1).In RAW264.7 macrophages,disrupted CX3CR1 signaling affected chemotaxis,potentially influencing immune cell migration in *** proteome analysis demonstrated the role of dysregulated immune cell migration in *** type-specific expression variations of these genes in the central nervous system(CnS),particularly microglia,were *** communication between neurons and glial cells was selectively altered in ALS *** integrated approach underscores m6A dysregulation in immune cells as a potential ALS contributor.

关键词： amyotrophic lateral sclerosis n^(6)-methyladenosine epi-transcriptome proteome single cell RnA sequencing analysis CX3CR1

FUT8-mediated aberrant n-glycosylation of SEMA7A promotes head and neck squamous cell carcinoma progression

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International Journal of Oral Science 2024年第2期16卷 333-348页

作者： Zhonglong liu Xiaoyan Meng Yuxin Zhang Jingjing Sun Xiao Tang Zhiyuan Zhang liu liu Yue He Department of Oral Maxillofacial&Head and neck Oncology Shanghai Ninth People’s Hospital Affiliated to Shanghai Jiao Tong University School of MedicineNational Clinical Research Center for Oral DiseaseShanghaiChina Department of Oral Surgery Shanghai Ninth People’s HospitalShanghai Jiao Tong University School of MedicineCollege of StomatologyShanghai Jiao Tong UniversityNational Center for StomatologyNational Clinical Research Center for Oral DiseasesShanghaiChina Department of Oral Pathology Shanghai Ninth People’s Hospital Affiliated to Shanghai Jiao Tong University School of MedicineNational Clinical Research Center for Oral Disease ShanghaiShanghaiChina

SEMA7A belongs to the Semaphorin family and is involved in the oncogenesis and tumor *** glycosylation has been intricately linked with immune escape and tumor ***7A is a highly glycosylated protein with five glycosylated *** underlying mechanisms of SEMA7A glycosylation and its contribution to immunosuppression and tumorigenesis are ***,we identify overexpression and aberrant n-glycosylation of SEMA7A in head and neck squamous cell carcinoma,and elucidate fucosyltransferase FUT8 catalyzes aberrant core fucosylation in SEMA7A at n-linked oligosaccharides(Asn 105,157,258,330,and 602)via a direct protein‒protein interaction.A glycosylated statue of SEMA7A is necessary for its intra-cellular trafficking from the cytoplasm to the *** EGF triggers SEMA7A n-glycosylation through increasing the binding affinity of SEMA7A toward FUT8,whereas TGF-β1 promotes abnormal glycosylation of SEMA7A via induction of epithelial–mesenchymal *** n-glycosylation of SEMA7A leads to the differentiation of CD8^(+)T cells along a trajectory toward an exhausted state,thus shaping an immunosuppressive microenvironment and being resistant immunogenic cell *** of SEMA7A significantly improves the clinical outcome of EGFR-targeted and anti-PD-L1-based ***,we also define RBM4,a splice regulator,as a downstream effector of glycosylated SEMA7A and a pivotal mediator of PD-L1 alternative *** findings suggest that targeting FUT8-SEMA7A axis might be a promising strategy for improving antitumor responses in head and neck squamous cell carcinoma patients.

关键词： aberrant squamous SEMA

Continuous near-complete photocatalytic degradation of toluene by V/n-doped TiO_(2)loade d on honeycomb ceramics under UV irradiation

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Journal of Materials Science & Technology 2024年第7期174卷 188-194页

作者： Gang liu Lijuan Han Jingwei Wang Yongqiang Yang Zuoyan Chen Bilu liu Xingcai An Gansu natural Energy Institute Lanzhou 730046China Shenzhen Geim Graphene Center Tsinghua-Berkeley Shenzhen Institute&Institute of Materials ResearchTsinghua Shenzhen International Graduate SchoolTsinghua UniversityShenzhen 518055China Shenyang national Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016China

Photocatalytic degradation of volatile organic compounds(VOCs)is a significant applying aspect of *** the modulation of photocatalysts and the rational dispersion of them on supports are key for solar-driven VOC *** batch-type photoreactors have low efficiency while continuous-flow photoreactors suffer from the problem of incomplete removal of ***,aiming for continuous and complete degradation of toluene gas as the target contaminant,continuous-flow pho-tocatalytic degradation reactors were made by adhering the vanadium and nitrogen codoped TiO_(2)on honeycomb ceramics(V/n-TiO_(2)@HC)by a simple sol-gel *** such a reactor,the rich ordered pores in the HC accelerate mass transport of toluene,and the introduction of V/n dopants narrows the bandgap and widens the light absorption range of TiO_(2),together resulting in continuous and nearly-complete pho-tocatalytic degradation of *** unique and stable structure of HC allows the photocatalysts to be *** degradation rate of toluene gas can reach 97.8%,and after 24 rounds of photocatalytic degra-dation,there is still a degradation rate of 96.7%.The impacts of loading times and gaseous flow rate on the photocatalytic performance of V/n-TiO_(2)@HC are studied in *** study provides a practical so-lution for the continuous and complete photocatalytic degradation of VOCs and opens a new application field for HC.

关键词： Honeycomb ceramics V/n co-doped TiO_(2) Photocatalytic degradation Toluene gas Continuous and complete degradation