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Selective Hydrodeoxygenation of Lignin-Derived Vanillin via Hetero-Structured High-Entropy Alloy/Oxide Catalysts

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Energy & Environmental Materials 2024年第3期7卷 202-210页

作者： Yan Sun Kaili liang Ren Tu Xudong Fan Charles Q.Jia Zhiwen Jia Yingnan Li hui Yang Enchen Jiang Hanwen Liu Yonggang Yao Xiwei Xu Key laboratory for Biobased Materials and Energy of Ministry of Education College of Materials and EnergySouth China Agricultural UniversityGuangzhou 510640China Department of Chemical Engineering and Applied chemistry University of Toronto200 College StreetToronto ON M5S3E5Canada State Key laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074China

The chemoselective hydrodeoxygenation of natural lignocellulosic materials plays a crucial role in converting biomass into value-added *** their complex molecular structures often require multiple active sites synergy for effective activation and achieving high ***,it is reported that a high-entropy alloy(HEA)on high-entropy oxide(HEO)hetero-structured catalyst for highly active,chemoselective,and robust vanillin *** heterogenous HEA/HEO catalysts were prepared by thermal reduction of senary HEOs(NiZnCuFeAlZrO_(x)),where exsolvable metals(e.g.,Ni,Zn,Cu)in situ emerged and formed randomly dispersed HEA nanoparticles anchoring on the HEO *** catalyst exhibits excellent catalytic performance:100%conversion of vanillin and 95%selectivity toward high-value 2-methyl-4 methoxy phenol at low temperature of 120℃,which were attributed to the synergistic effect among HEO matrix(with abundant oxygen vacancies),anchored HEA nanoparticles(having excellent hydrogenolysis capability),and their intimate hetero-interfaces(showing strong electron transferring effect).Therefore,our work reported the successful construction of HEA/HEO heterogeneous catalysts and their superior multifunctionality in biomass conversion,which could shed light on catalyst design for many important reactions that are complex and require multifunctional active sites.

关键词： biomass conversion heterogeneous catalysts high-entropy oxide high-entropy alloys lignin pyrolysis

Oxygen vacancy promoting artificial atom(RuPd)by d-orbital coupling for efficient water dissociation

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Nano Research 2024年第8期17卷 7045-7052页

作者： Ruofan Shen Yanyan Liu Shuling Liu Shuyan Guan Huanhuan Zhang Sehrish Mehdi Saima Ashraf Ting-hui Xiao Erjun liang Jianchun Jiang Yongfeng Wang Baojun Li laboratory of Zhongyuan Light School of PhysicsZhengzhou UniversityZhengzhou 450001China Key laboratory of Materials Physics Ministry of EducationSchool of PhysicsZhengzhou UniversityZhengzhou 450001China college of chemistry Zhengzhou UniversityZhengzhou 450001China college of Science Henan Agricultural UniversityZhengzhou 450002China Department of chemistry Tsinghua UniversityBeijing 100084China National Engineering lab.for Biomass Chemical Utilization Institute of Chemical Industry of Forest ProductsCAFNanjing 210042China Center for Carbon-based electronics and Key laboratory for the Physics and chemistry of Nanodevices Department of ElectronicsPeking UniversityBeijing 100871China

Rational design of highly active catalysts for breaking hydrogen-oxygen bonds is of great significance in energy chemical reactions involving ***,an efficient strategy for the artificial atom(RuPd)established by d-orbital coupling and adjusted by oxygen vacancy(V_(O))is verified for water *** an experimental verification,the turnover frequency of RuPd-TiO_(2)-VO(RuPdTVO)catalyst in ammonia borane hydrolysis reaches up to 2750 min^(−1)(26,190 min−1 based on metal dispersion)in the absence of alkali,exceeding the highest active catalysts(Rh-based catalysts).The d-orbital coupling effect between Ru and Pd simulates the outer electronic structure of *** transfer from V_(O) to(RuPd)constructs an electron-rich state of active sites that further enhances the ability of the artificial atom to dissociate *** work provides an effective electronic regulation strategy from V_(O) and artificial atom constructed by d-orbital coupling effect for efficient water dissociation.

关键词： ammonia borane hydrolysis d-orbital coupling oxygen vacancy artificial atom water dissociation

The RNA binding protein EHD6 recruits the m^(6)A reader YTH07 and sequesters OsCOL4 mRNA into phase-separated ribonucleoprotein condensates to promote rice flowering

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molecular Plant 2024年第6期17卷 935-954页

作者： Song Cui Peizhe Song Chaolong Wang Saihua Chen Benyuan Hao Zhuang Xu liang Cai Xu Chen Shanshan Zhu Xiangchao Gan hui Dong Yuan Hu liang Zhou Haigang Hou Yunlu Tian Xi Liu liangming Chen Shijia Liu Ling Jiang Haiyang Wang Guifang Jia Shirong Zhou Jianmin Wan State Key laboratory for Crop Genetics&Germplasm Enhancement and Utilization Zhongshan Biological Breeding LaboratoryNational Observation and Research Station of Rice Germplasm ResourcesNanjing Agricultural UniversityNanjing 210095China State Key laboratory for Crop Gene Resources and Breeding Institute of Crop ScienceChinese Academy of Agricultural SciencesBeijing 100081China Synthetic and Functional Biomolecules Center Beijing National Laboratory for Molecular SciencesKey Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking-Tsinghua Center for Life SciencesBeijing Advanced Center of RNA BiologyPeking UniversityBeijingChina Jiangsu Key laboratory of Crop Genomics and molecular Breeding Agricultural College of Yangzhou UniversityYangzhou 225009China Max Planck Institute for Plant Breeding Research Carl-von-Linne´-Weg 1050829 KolnGermany

N6-Methyladenosine(m^(6)A)is one of the most abundant modifications of eukaryotic mRNA,but its comprehensive biological functionality remains further *** this study,we identified and characterized a new flowering-promoting gene,EARLY HEADING DATE6(EHD6),in ***6 encodes an RNA recognition motif(RRM)-containing RNA binding protein that is localized in the non-membranous cytoplasm ribonucleoprotein(RNP)granules and can bind both m^(6)A-modified RNA and unmodified RNA *** found that EHD6 can physically interact with YTH07,a YTH(YT521-B homology)domain-containing m^(6)A *** showed that their interaction enhances the binding of an m^(6)A-modified RNA and triggers relocation of a portion of YTH07 from the cytoplasm into RNP granules through phase-separated *** these condensates,the mRNA of a rice flowering repressor,CONSTANS-like 4(OsCOL4),becomes sequestered,leading to a reduction in its protein abundance and thus accelerated flowering through the Early heading date 1 *** together,these results not only shed new light on the molecular mechanism of efficient m^(6)A recognition by the collaboration between an RNA binding protein and YTH family m^(6)A reader,but also uncover the potential for m^(6)A-mediated translation regulation through phaseseparated ribonucleoprotein condensation in rice.

关键词： N6-methyladenosine m^(6)A EHD6 YTH domain-containing protein phase separation heading date

What Can Topology Bring to chemistry?

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CCS chemistry 2024年第9期6卷 2084-2109页

作者： Wei Wang Songtao Zhou Xiujun Yu Qing-hui Guo Yanhang Ma Jie Song liang Zhang Xuzhou Yan Lu Han Qing Liao Xiaopeng Li Wen-Bin Zhang Yiyong Mai Shaodong Zhang Shunai Che Hai-Bo Yang Xuefeng Fu Mei-Xiang Wang school of chemistry and molecular Engineering East China Normal UniversityShanghai 200062 Hangzhou Institute of Medicine Chinese Academy of SciencesHangzhou 310022Zhejiang college of chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060Guangdong MOE Key laboratory of Bioorganic Phosphorous and Chemical Biology Department of ChemistryTsinghua UniversityBeijing 100084 school of Physical Science and Technology and Shanghai Key laboratory of High-Resolution electron Microscopy ShanghaiTech UniversityShanghai 201210 school of chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesState Key Laboratory of Composite MaterialsShanghai Key Laboratory for Molecular Engineering of Chiral DrugsShanghai Jiao Tong UniversityShanghai 200240 school of Chemical Science and Engineering Tongji UniversityShanghai 200092 Beijing Key laboratory for Optical Materials and Photonic Devices Department of ChemistryCapital Normal UniversityBeijing 100048 Beijing National laboratory for molecular sciences Key Laboratory of Polymer Chemistry and Physics of Ministry of EducationCenter for Soft Matter Science and EngineeringCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871 Department of Chemical sciences National Natural Science Foundation of ChinaBeijing 10085

The unique mathematical perspectives and principal concepts of topology have not only promoted the development of other branches of mathematics but have also deeply influenced other subjects,particularly physics and *** minireview aims to elucidate the substantial influence of topology on chemistry by critically examining both the contributions of topology to current chemical science and its potential future *** will discuss the topology of molecular structures and assemblies across various scales—from small molecules and mechanically interlocked molecules to polymers,biomacromolecules,and supramolecular *** discussion will include an exploration of cutting-edge techniques for characterizing topological features,underscoring the role of topology as a novel paradigm for the design and synthesis of new molecular ***,a critical analysis of topology’s role in the development of functional materials—such as photonic materials,polymers,biomacromolecules,and chiral materials—will demonstrate its emerging significance as a crucial parameter in unveiling novel properties and *** topology’s formidable potential,it is anticipated to be used increasingly to address pivotal challenges within chemistry and adjacent disciplines.

关键词： chemical topology topological invariants molecular graphs links and knots structureproperty relationship

MOFs‑Derived Strategy and Ternary Alloys Regulation in Flower‑Like Magnetic‑Carbon Microspheres with Broadband Electromagnetic Wave Absorption

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Nano-Micro Letters 2024年第11期16卷 479-493页

作者： Mengqiu Huang Bangxin Li Yuetong Qian Lei Wang huibin Zhang Chendi Yang Longjun Rao Gang Zhou Chongyun liang Renchao Che laboratory of Advanced Materials Shanghai Key Lab of Molecular Catalysis and Innovative MaterialsAcademy for Engineering&TechnologyFudan UniversityShanghai 200438People’s Republic of China Department of chemistry Fudan UniversityShanghai 200438People’s Republic of China Materials Genome Institute Shanghai UniversityShanghai 200444People’s Republic of China school of Materials Science and Engineering Shanghai Institute of TechnologyShanghai 201418People’s Republic of China college of Physics Donghua UniversityShanghai 201620People’s Republic of China Zhejiang laboratory Hangzhou 311100People’s Republic of China

Broadband electromagnetic(EM)wave absorption materials play an important role in military stealth and health ***,metal–organic frameworks(MOFs)-derived magnetic-carbon CoNiM@C(M=Cu,Zn,Fe,Mn)microspheres are fabricated,which exhibit flower-like nano–microstructure with tunable EM response *** on the MOFs-derived CoNi@C microsphere,the adjacent third element is introduced into magnetic CoNi alloy to enhance EM wave absorption *** term of broadband absorption,the order of efficient absorption bandwidth(EAB)value is Mn>Fe=Zn>Cu in the CoNiM@C ***,MOFs-derived flower-like CoNiMn@C microspheres hold outstanding broadband absorption and the EAB can reach up to 5.8 GHz(covering 12.2–18 GHz at 2.0 mm thickness).Besides,off-axis electron holography and computational simulations are applied to elucidate the inherent dielectric dissipation and magnetic *** heterointerfaces in CoNiMn@C promote the aggregation of the negative/positive charges at the contacting region,forming interfacial *** graphitized carbon layer catalyzed by the magnetic CoNiMn core offered the electron mobility path,boosting the conductive *** importantly,magnetic coupling is observed in the CoNiMn@C to strengthen the magnetic responding *** study provides a new guide to build broadband EM absorption by regulating the ternary magnetic alloy.

关键词： Magnetic-carbon microspheres MOFs derivatives Electromagnetic wave absorption Magnetic loss Broadband absorption

以密度泛函论与局域近似法及改进过渡态计算软硬度

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西南师范大学学报（自然科学版） 2005年第1期30卷 108-112页

作者：张梦军覃仁辉黄莺李志良第三军医大学检验系重庆400038 重庆大学化学化工学院应用化学系重庆400044 湖南中医学院药学分院湖南长沙410007

应用密度泛函论(DFT)及其局域近似法(LDA)、局域近似法加全域性校正(LDB: LDA GCE)和改进斯莱特过渡态法(MST), 并依能量型标度定义, 采用有限差分法(DDM), 同时考虑相对论效应, 对元素电离能 P和电子亲合能Q 及原子软硬度U等进行精确... 详细信息

应用密度泛函论(DFT)及其局域近似法(LDA)、局域近似法加全域性校正(LDB: LDA GCE)和改进斯莱特过渡态法(MST), 并依能量型标度定义, 采用有限差分法(DDM), 同时考虑相对论效应, 对元素电离能 P和电子亲合能Q 及原子软硬度U等进行精确估计与理论预测. 把计算扩展到全部 112 种元素, 计算值相当文献值水平或优于其它近似泛函法, 更接近实验值. 该U值在分子模建与设计等方面将获广泛应用.

关键词：软硬度元素电离能电子亲合能密度泛函理论局域密度近似全域性校正改进过渡态法有限差分法

Super-assembly of integrated gold magnetic assay with loopmediated isothermal amplification for point-of-care testing

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Nano Research 2023年第1期16卷 1242-1251页

作者： Jianping liang Jie Zeng Xiaojuan Huang Tengteng Zhu Yonglong Gong Chen Dong Xiangrong Wang Lingzhi Zhao Lei Xie Kang liang Qiongxiang Tan Yali Cui Biao Kong Wenli hui The college of life science Northwest UniversityXi’an 710069China Shaanxi Provincial Engineering Research Center for Nano-Biomedical Detection Xi’an 710077China Department of chemistry Shanghai Key Lab of Molecular Catalysis and Innovative MaterialsCollaborative Innovation Center of Chemistry for Energy MaterialsFudan UniversityShanghai 200438China Key laboratory of Resource Biology and Biotechnology in Western china Ministry of EducationNorthwest UniversityXi’an 710069China Provincial Key laboratory of Biotechnology of Shaanxi Province Northwest UniversityXi’an 710069China school of Chemical Engineering Graduate School of Biomedical Engineeringand Australian Centre for NanoMedicineUniversity of New South WalesNSW 2052Australia

With the increasing global threat of various diseases and infections,it is essential to develop a fast,low-cost,and easy-to-use point-of-care testing(POCT)system for inspections at all levels of medical institutions and self-examination at *** this work,gold magnetic nanoparticles(GMNPs)are used as the key material,and a rapid visual detection method is designed through integrating loop-mediated isothermal amplification(LAMP)and lateral flow assay(LFA)biosensor for detecting a variety of analytes which includes whole blood,buccal swabs,and *** is worth to note that the proposed method does not need DNA ***,uracil DNA glycosylase(UDG)is employed to eliminate carrier contamination for preventing false positive *** whole detection process can be finished within 25 *** accuracy of detection is measured by assessing the polymorphisms of the methylenetetrahydrofolate reductase(MTHFR)*** detection limit of the newly developed extraction-free detection system for MTHFR C677T is 0.16 ng/μL.A preliminary clinical study of the proposed method is carried out by analyzing 600 clinical samples(including 200 whole blood samples,100 buccal swabs,and 300 genomic DNA samples).The results indicate that the proposed method is 100%consistent with the sequencing results which provides a new choice for POCT and shows a broad application prospect in all levels of medical clinics and at home.

关键词： gold magnetic nanoparticles loop-mediated isothermal amplification lateral flow assay system free extraction singlenucleotide polymorphisms genotyping

Cobalt/nitrogen co-carved carbon nanorod for efficient Fenton-like reaction:Degradation efficacy,reaction mechanism and singlet oxygen generation

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Journal of Materials Science & Technology 2023年第6期137卷 67-78页

作者： Meng Li Ke Zheng Yu-Ting Jin Zhao-Xin Zhang Ji-liang Cheng Long-Wei Huang Ce-hui Mo Shao-Qi Zhou Guangdong Provincial Research Center for Environment Pollution Control and Remediation Materials College of Life Science and TechnologyJinan UniversityGuangzhou 510632China college of Environment and Energy Guangzhou Higher Education Mega CentreSouth China University of TechnologyGuangzhou 510006China Department of Chemical and Biological Engineering The Hong Kong University of Science and TechnologyClear Water BayKowloonHong Kong SARChina school of Civil Engineering and Transportation South China University of TechnologyGuangzhou 510640China Thrust of Sustainable Energy&Environment The Hong Kong University of Science and TechnologyGuangzhou 511458China college of Resources and Environmental Engineering Guizhou UniversityGuiyang 550025China

The Fenton-like process shows promising potential to generate reactive oxygen species for the reme-diation of increasingly environmental ***,the slow development of high-activity cata-lysts with strong stability and low leaching of metal ions has greatly inhibited scale-up application of this ***,cobalt(Co)/nitrogen(N)atom co-curved carbon nanorod(CoNC)containing highly uniform CoN_(x)active sites is developed as a Fenton-like catalyst for the effective catalytic oxidation of various organics via peroxymonosulfate(PMS)activation with high *** confirmed by the exper-imental results,singlet oxygen(^(1)O_(2))is the dominant active species for the degradation of the organ-ics,with a proportion of 100%.Furthermore,density functional theory calculations indicate that CoN_(2)C_(2)is the most effective ligand structure with more negative adsorption energy for PMS and the shortest length Co-O bond,while the most reasonable generation pathway for^(1)O_(2)was CoN_(2)C_(2)-PMS→CoN_(2)C_(2)-OH∗→2O∗→^(1)O_(2).Further studies demonstrate that the electron can be transferred from the highest occupied molecular orbitals of the organics to the lowest unoccupied molecular orbitals of the PMS via CoN_(2)C_(2)*** addition,the CoNC presents strong resistance to inorganic ions and natural organic matter in the Fenton-like catalysis *** presence of CoN_(2)C_(2)active centre can significantly shorten the migration distance of the^(1)O_(2)generated from PMS activation,which further enhances the Fenton-like catalytic activity in terms of mineralising various organic contaminants with high efficiency over a wide pH range.

关键词： Non-radical pathway Singlet oxygen Co/N co-carved carbon nanorod Fenton-like catalysis

Super-assembled sandwich-like Au@MSN@Ag nanomatrices for high-throughput and efficient detection of small biomolecules

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Nano Research 2022年第3期15卷 2722-2733页

作者： Dantong Zhao Chunxia Ma Meng Gao Yong Li Bo Yang hui Li Runhao Zhang Minglu Hao Jing Huang Kang liang Pu Chen Lei Xie Rong Rong Biao Kong college of Medicine Shandong University of Traditional Chinese MedicineJinan 250355China Shandong Analysis and Test Center National Supercomputer Research Center of Advanced MaterialsAdvanced Materials InstituteQilu University of Technology(Shandong Academy of Sciences)Jinan 250014China Heze Institute for Food and Drug Control Heze 274000China school of Chemical Engineering and Graduate school of Biomedical Engineering The University of New South WalesNSW 2052Australia Department of Chemical Engineering University of WaterlooWaterlooOntarioN2L 3G1Canada Department of chemistry Shanghai Key Lab of Molecular Catalysis and Innovative MaterialsiChEMFudan UniversityShanghai 200032China

Small biomolecules(m/z<500)are the material basis of organisms and participate in life activities,but their comprehensive and accurate detection in complex samples remains a ***-assisted laser desorption/ionization ma... 详细信息

Small biomolecules(m/zmolecular analysis with high *** development of a new matrix is essential to improve the efficiency of the MALDI-MS for molecular compound *** this work,the sandwich-like gold nanoparticles@mesoporous silica nanocomposite@silver nanoparticles(Au@MSN@Ag)nanospheres were prepared by layer-by-layer super-assembly strategy,and can be used as a novel matrix for the quantitative detection and enrichment of small biomolecules by *** sandwich-like nanospheres form a unique plasma resonant cavity that effectively absorbs the laser energy,while the homogeneous mesoporous structure of MSN can lock the analyte,which is essential for efficient LDI of small *** to traditional matrices,Au@MSN@Ag shows the advantages of low background,wide application range,high sensitivity,super high salt and protein tolerance,and good *** example,the detection limit of glucose was as low as 5 fmol,and showed a good linear relationship in the range of 1−750μg/***@MSN@Ag assisted LDI-MS allows the enrichment and detection of small molecules in traditional Chinese medicine(TCM)without derivatization and purification,classification of herbs using the accurate quantitative results oligosaccharides,and identification of gelatin by amino acid *** research could help in designing more efficient nanostructure matrices and further explored the application of LDI-MS.

关键词： matrix-assisted laser desorption/ionization mass spectrometry(MALDI-MS) matrix sandwich-like nanostructures small biomolecules traditional Chinese medicine(TCM)