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Confined Mn^(2+) enables effective aerobic oxidation catalysis

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Science China Chemistry 2024年第5期67卷 1545-1553页

作者： Desheng Yuan Sicong Ma Xiao Kong Chi Zhang lin Chen Chengsheng Yang Lihua Wang Zhen Liu lin ye Yongmei Liu Rui Ma Zhi-Pan Liu Yifeng Zhu Yong Cao Xinhe Bao Department of Chemical Physics University of Science and Technology of ChinaHefei 230026China Department of Chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsCollaborative Innovation Center of Chemistry for Energy MaterialsFudan UniversityShanghai 200438China Key Laboratory of Synthetic and Self-Assembly Chemistry for Organic Functional Molecules Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China School of Materials and Chemistry University of Shanghai for Science and TechnologyShanghai 200093China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China Institute of Advanced Fluorine-Containing Materials Zhejiang Normal UniversityJinhua 321004China State Key Laboratory of Catalysis National Laboratory for Clean EnergyCollaborative Innovation Center of Chemistry for Energy MaterialsDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

Effective and mild activation of O_(2) is essential but challenging for aerobic oxidation. In heterogeneous catalysis, high-valence manganese oxide(e.g., +4) is known to be active for the oxidation, whereas divalent MnO is ineffective due to its limited capacity to supply surface oxygen and its thermodynamically unstable structure when binding O_(2) in reaction conditions. Inspired by natural enzymes that rely on divalent Mn^(2+), we discovered that confining Mn^(2+) onto the Mn_(2)O_(3) surface through a dedicated calcination process creates highly active catalysts for the aerobic oxidation of 5-hydroxymethylfurfural, benzyl alcohol, and *** Mn_(2)O_(3)-confined Mn^(2+) is undercoordinated and efficiently mediates O_(2) activation, resulting in 2–3 orders of magnitude higher activity than Mn_(2)O_(3) alone. Through low-temperature infrared spectroscopy, we distinguished low-content Mn^(2+) sites at Mn_(2)O_(3) surface, which are difficult to be differentiated by X-ray photoelectron spectroscopy. The combination of in-situ energydispersive X-ray absorption spectroscopy and X-ray diffraction further provides insights into the formation of the newly identified active Mn^(2+) sites. By optimizing the calcination step, we were able to increase the catalytic activity threefold *** finding offers promising frontiers for exploring active oxidation catalysts by utilizing the confinement of Mn^(2+)and oftenignored calcination skills.

关键词： confinement catalysis manganese oxide aerobic oxidation divalent Mn^(2+) operando spectroscopies

Insights into therapeutic peptides in the cancerimmunity cycle:Update and challenges

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Acta Pharmaceutica Sinica B 2024年第9期14卷 3818-3833页

作者： Xiaokun Zhang ye Wu Jiayi lin Shengxin Lu Xinchen Lu Aoyu Cheng Hongzhuan Chen Weidong Zhang Xin Luan Shanghai Frontiers Science Center for Chinese Medicine Chemical Biology Institute of Interdisciplinary Integrative Medicine Research and Shuguang HospitalShanghai University of Traditional Chinese MedicineShanghai 201203China Institute of Medicinal Plant Development Chinese Academy of Medical Science&Peking Union Medical CollegeBeijing 100193China School of Pharmacy Second Military Medical UniversityShanghai 200433China Department of Pharmacology School of PharmacyFudan UniversityShanghai 201203China

Immunotherapies hold immense potential for achieving durable potency and long-term survival opportunities in cancer *** vital biological mediators,peptides with high tissue penetration and superior selectivity offer significant promise for enhancing cancer immunotherapies(CITs).However,physicochemical peptide features such as conformation and stability pose challenges to their on-target *** review provides a comprehensive overview of recent advancements in therapeutic peptides targeting key steps of the cancer-immunity cycle(CIC),including tumor antigen presentation,immune cell regulation,and immune checkpoint *** attention is given to the opportunities and challenges associated with these peptides in boosting CIC within the context of clinical ***,possible future developments in this field are also discussed to provide insights into emerging CITs with robust efficacy and safety profiles.

关键词： Cancer-immunity cycle Oncolytic peptide Peptide neoantigen vaccine Peptide mimotope Immune checkpoint blockade Cancer immunotherapy Synthetic long peptide vaccine Peptide-major histocompatibility complex

Nanosize-effect on the distribution of heavy metals in copper smelting dust:Based on sophisticated dust sorting approach

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Nano Research 2024年第1期17卷 312-320页

作者： Ken Li Zuwu Liao Hengdi ye Qingzhu Li Fenghua Shen Qian Li Hui Liu Qingwei Wang Xu Yan Zhang lin Liyuan Chai School of Metallurgy and Environment Central South UniversityChangsha 410083China Chinese National Engineering Research Center for Control&Treatment of Heavy Metal Pollution Changsha 410083China National Engineering Research Center of Sintering and Pelletizing Equipment System Zhongye Changtian International Engineering Co.LtdChangsha 410205China

Dust particles emitted from smelters can be hazardous to ecosystems and humans,as they are often enriched in metallic ***,we combined multi-method mineralogical analysis with a sophisticated size sorting approach for copper smelting dust to study the nanosize-effect on heavy metal distribution,which has hitherto been *** types of dust were collected from a copper flash smelter and then size-sorted using a Dekati low-pressure *** showed that all three samples could easily sort out nanoscale dust particles(sence of heavy metals(Pb,Zn,Cu,and As)and their mineral species in dust was examined at various particle *** was discovered that different heavy metals are enriched on nanoparticles in specific *** micron-sized particles,heavy metals are generally found in discrete phases(e.g.,CuSO_(4),PbSO_(4),and As_(2)O_(3)).In nanoscale particles,the dominant phase is Fe_(3)O_(4),while heavy metals are mostly found in lattice substitution(e.g.,CuFe_(2)O_(4)and ZnFe_(2)O_(4)).Two distinct nano-dust morphologies were found:One with irregular mesh or chain structures consisting of particles of a few nanometers,and the other with polygonal crystals in larger sizes of hundreds of *** enrichment of heavy metals in the latter morphology is more pronounced,possibly because lattice substitution of heavy metals is more likely to occur when polycrystalline particles are formed.

关键词： copper flue dust size-sorted heavy metal distribution morphology nano-sized effects

TiO_(2)Electron Transport Layer with p-n Homojunctions for Efficient and Stable Perovskite Solar Cells

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Nano-Micro Letters 2024年第10期16卷 1-14页

作者： Wenhao Zhao Pengfei Guo Jiahao Wu Deyou lin Ning Jia Zhiyu Fang Chong Liu Qian ye Jijun Zou Yuanyuan Zhou Hongqiang Wang State Key Laboratory of Solidification Processing Center for Nano Energy MaterialsSchool of Materials Science and EngineeringNorthwestern Polytechnical University and Shaanxi Joint Laboratory of Graphene(NPU)Xi'an 710072People's Republic of China Department of Chemical and Biological Engineering Hong Kong University of Science and TechnologyClear Water BayHong Kong SARPeople's Republic of China Key Laboratory for Green Chemical Technology of the Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072People's Republic of China Chongqing Innovation Center of Northwestern Polytechnical UniversityNorthwestern Polytechnical UniversityChongqing 401135People's Republic of China

Low-temperature processed electron transport layer(ETL)of TiO_(2)that is widely used in planar perovskite solar cells(PSCs)has inherent low carrier mobility,resulting in insufficient photogenerated elec-tron transport and thus recombination loss at buried ***,we demonstrate an effective strategy of laser embedding of p-n homojunctions in the TiO_(2)ETL to accelerate electron transport in PSCs,through localized build-in electric fields that enables boosted electron mobility by two orders of *** embedding is found significantly helpful for not only the enhanced crystallization quality of TiO_(2)ETL,but the fabrication of perovskite films with larger-grain and the *** embedded p-n homojunction enables also the modulation of interfacial energy level between perovskite layers and ETLs,favoring for the reduced voltage deficit of *** from these merits,the formamidinium lead iodide(FAPbI_(3))PSCs employing such ETLs deliver a champion efficiency of 25.50%,along with much-improved device stability under harsh conditions,i.e.,maintain over 95%of their initial efficiency after operation at maximum power point under continuous heat and illumination for 500 h,as well as mixed-cation PSCs with a champion efficiency of 22.02%and over 3000 h of ambient storage under humidity stability of 40%.Present study offers new possibilities of regulating charge transport layers via p-n homojunction embedding for high performance optoelectronics.

关键词： Electron transport layer p-n homojunction Electron mobility Buried interface Perovskite solar cells

Oxygen‑Coordinated Single Mn Sites for Efficient Electrocatalytic Nitrate Reduction to Ammonia

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Nano-Micro Letters 2024年第1期16卷 147-159页

作者： Shengbo Zhang Yuankang Zha Yixing ye Ke Li Yue lin Lirong Zheng Guozhong Wang Yunxia Zhang Huajie Yin Tongfei Shi Haimin Zhang Laboratory of Materials Physics Centre for Environmental and Energy NanomaterialsAnhui Key Laboratory of Nanomaterials and NanotechnologyCAS Center for Excellence in NanoscienceInstitute of Solid State PhysicsHFIPSChinese Academy of SciencesHefei 230031People’s Republic of China University of Science and Technology of China Hefei 230026People’s Republic of China Key Laboratory of Agricultural sensors Ministry of AgricultureSchool of Information and ComputerAnhui Agricultural UniversityHefei 230026People’s Republic of China Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026People’s Republic of China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of Sciences19B Yuquan RoadBeijing 100049People’s Republic of China

Electrocatalytic nitrate reduction reaction has attracted increasing attention due to its goal of low carbon emission and environmental ***,we report an efficient NitRR catalyst composed of single Mn sites with atomically dispersed oxygen(O)coordination on bacterial cellulose-converted graphitic carbon(Mn-O-C).Evidence of the atomically dispersed Mn-(O-C_(2))_(4)moieties embedding in the exposed basal plane of carbon surface is confirmed by X-ray absorption *** a result,the as-synthesized Mn-O-C catalyst exhibits superior NitRR activity with an NH_(3)yield rate(RNH_(3))of 1476.9±62.6μg h^(−1)cm^(−2)at−0.7 V(*** hydrogen electrode,RHE)and a faradaic efficiency(FE)of 89.0±3.8%at−0.5 V(***)under ambient ***,when evaluated with a practical flow cell,Mn-O-C shows a high RNH_(3)of 3706.7±552.0μg h^(−1)cm^(−2)at a current density of 100 mA cm−2,2.5 times of that in the H *** in situ FT-IR and Raman spectroscopic studies combined with theoretical calculations indicate that the Mn-(O-C_(2))_(4)sites not only effectively inhibit the competitive hydrogen evolution reaction,but also greatly promote the adsorption and activation of nitrate(NO_(3)^(−)),thus boosting both the FE and selectivity of NH_(3)over Mn-(O-C_(2))_(4)sites.

关键词： Atomically dispersed Oxygen coordination Nitrate reduction reaction In situ spectroscopic studies Hydrogen evolution reaction

Analysis and Characterization of the GABA Transaminase and Succinate Semialdehyde Dehydrogenase Genes in the Microalga Isochrysis zhanjiangensis in Response to Abiotic Stresses

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Journal of Ocean University of China 2024年第3期23卷 775-785页

作者： TIAN Jiaojiao ZHANG lin LU Xinyue ye lingzhi WU Yuanyuan CHEN Deshui CAO Jiayi JIANG Jiaxin XU Jilin YAN Xiaojun Key Laboratory of Marine Biotechnology of Zhejiang Province School of Marine SciencesNingbo UniversityNingbo 315211China Key Laboratory of Aquacultural Biotechnology Ministry of Education Ningbo UniversityNingbo 315211China Laizhou Bay Marine Technology Co. Ltd.Yantai 261400China Fujian Dalai Seed Science and Technology Co. Ltd.Ningde 352101China

Gamma-aminobutyric acid(GABA),widely existing in different organisms,is rapidly accumulated in plants in response to environmental *** main biosynthesis and degradation pathways of GABA constitute the GABA shunt,which is tied to the tricarboxylic acid(TCA)*** transaminase(GABA-T)and succinate semialdehyde dehydrogenase(SSADH)are two essential enzymes for the GABA degradation *** there are abundant studies on GABA shunt in higher plants at the physiological and genetic levels,research on its role in microalgae remains *** study aimed at exploring the function of GABA-T and SSADH genes in Isochrysis zhanjiangensis,an important diet microalga,under different *** cloned two GABA-T genes,IzGABA-T1 and IzGABA-T2,and one SSADH gene IzSSADH from Isochrysis zhanjiangensis and conducted heterologous expression *** results showed that the overexpression of IzGABA-T1 or IzGABA-T2 enhanced the survival rates of yeast transformants under heat or NaCl stress,while the overexpression of IzSSADH improved yeast tolerance to NaCl stress but had no obvious effect on heat ***,the results of quantitative real-time polymerase chain reaction(qPCR)showed that IzGABA-T1 transcription increased in the HT(salinity 25,35℃)and LS(salinity 15,25℃)*** 24 h,the IzGABA-T2 transcriptions increased in the HT,LS,and HS(salinity 35,25℃)groups,but their transcription levels decreased in all groups at 48 *** transcription increased in the LS *** results suggest that IzGABA-T1,IzGABA-T2,and IzSSADH are associated with temperature and salinity stresses and possess a certain preference for different stresses.

关键词： abiotic stress GABA heterologous expression Isochrysis zhanjiangensis transcription

Sperm acrosin activity may be a useful factor in choosing between ICSI and IVF for infertile male patients

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Asian Journal of Andrology 2024年第1期26卷 85-90页

作者： ye-Na Hu Liang Hu Xin-Yu Yin Huan Zhang Yang-Qin Peng Gang Liu Ge lin Wei-Na Li The Institute of Reproductive and Stem Cell Engineering School of Basic Medical ScienceCentral South UniversityChangsha 410008China Department of Andrology Reproductive and Genetic Hospital of CITiC-XiangyaChangsha 410013China Clinical Research Center for Reproduction and Genetics in Hunan Province Changsha 410013China Hunan Guangxiu Hi-tech Life Technology Co. Ltd.Changsha 410013China

The clinical applications of acrosin activity are *** analyzed 61578 male partners in infertile couples who visited the outpatient department of the Reproductive and Genetic Hospital of CITIC-Xiangya(Changsha,China)between August 2014 and December 2019 to determine the reference ranges and thresholds for acrosin activity in infertile Chinese men;to determine whether correlations exist between acrosin activity and age,sperm concentration,sperm morphology,or sperm motility;and to evaluate whether acrosin activity could serve as an effective prognostic indicator for choosing between in vitro fertilization(IvF)and intracytoplasmic sperm injection(icsl)in the *** cut-off value for the normal reference range of acrosin activity for male partners in infertile couples was 24.78μlU per 106 *** was no significant association between acrosin activity and age,sperm concentration,semen volume,total sperm count,progressive motility,or total motile spermatozoa.A weak positive correlation was found between acrosin activity and normal sperm *** was a statistically significant difference in abnormal acrosome morphology between the group with high acrosin activity(>24.78μlU per 106 sperm)and the group with low acrosin activity(<24.78μlU per 106 sperm).The group with a low IVF fertilization rate had a high index of abnormal acrosomal morphology at 21.2%,while the group with a high IVF fertilization rate had a low index of 0.2%.At an acrosin activity of<24.78μlU per 10 sperm,in one cycle of the same patient,the fertilization rate,normal fertilization rate,and good-quality embryo rate for Icsl were significantly higher than those for ***,the most promising application of acrosin activity could be in the selection of IcsI over IVF for infertile male patients with complete fertilization failure or a low fertilization rate.

关键词： acrosin activity fertilization rate ICSI IVF semen parameters

Pairs of thiol-substituted 1,2,4-triazole-based isomeric covalent inhibitors with tunable reactivity and selectivity

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Chinese Chemical Letters 2024年第7期35卷 329-335页

作者： Shiqi Xu Zi ye Shuang Shang Fengge Wang Huan Zhang Lianguo Chen Hao lin Chen Chen Fang Hua Chong-Jing Zhang State Key Laboratory of Bioactive Substance and Function of Natural Medicines Beijing Key Laboratory of Active Substance Discovery and Druggability EvaluationInstitute of Materia MedicaChinese Academy of Medical Sciences and Peking Union Medical CollegeBeijing 100050China State Key Laboratory of Bioactive Substance and Function of Natural Medicines Beijing Key Laboratory of New Drug Mechanisms and Pharmacological Evaluation Study(BZ0150)Institute of Materia MedicaPeking Union Medical College and Chinese Academy of Medical SciencesBeijing 100050China The First Affiliated Hospital of Wenzhou Medical University Wenzhou 325000China

Covalent bioactive compounds are successfully used in clinic and attracted intense research efforts in the fundamental study as well as drug *** advantageous effects of covalent compounds compared with non-covalent ones are highly dependent on electrophilic ***,electrophilic warheads with tunable reactivity and selectivity are highly demanded in fields of medicinal chemistry and chemical ***,we report a novel electrophilic warhead,chloromethyl group activated by thiol-substituted 1,2,***,a pair of regioisomers could be simultaneously occurred in the step of alkylation during the synthesis of this unique *** is a rare example that the alkylation could simultaneously generate these two separable regioisomers of 1,2,4-triazole at the nitrogen or sulfur *** covalent-working mechanism of this new warhead is confirmed by various chemoproteomics experiments including target identification and binding site ***,the reactivity and selectivity of this new electrophilic warhead could be efficiently tuned by virtue of stereo ***,one pair of regioisomers(19S and 19X)induced distinct modes of cell *** 19S could induce apoptosis of colon cancer cells while 19X could induce both apoptosis and ***,this study provides pairs of novel electrophilic warheads that could be useful not only in supporting the design of covalent compounds for drug discovery but also in providing chemical probes for the fundamental biological study.

关键词： Electrophilic warhead Covalent inhibitor 1,2,4-Triazole Chemical proteomics GSTO1

The First Ground-based White Light Lunar Polarization Imaging:A New Kind of FeO Observation on the Near Side of the Moon

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Research in Astronomy and Astrophysics 2024年第6期24卷 1-6页

作者： Wei-Nan Wang Jin-Song Ping Ming-Yuan Wang Wen-Zhao Zhang Han-lin ye Xing-Wei Han Song-Feng Kou Changchun Observatory National Astronomical ObservatoriesChinese Academy of SciencesChangchun 130117China National Astronomical Observatories Chinese Academy of SciencesBeijing 100101China University of Chinese Academy of Sciences Beijing 101408China Astronomy Department Beijing Normal UniversityBeijing 100875China International Center for Climate and Environment Sciences Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China Nanjing Institute of Astronomical Optics and Technology Chinese Academy of SciencesNanjing 210042China

Lunar optical polarization is a fascinating phenomenon that occurs when sunlight reflects off the surface of the Moon and becomes *** study employs a novel split-focus plane polarimetric camera to conduct the initial white light polarimetric observations on the near side of the *** obtained the linear degree of polarization(DOP)parameters of white light by observation from the eastern and western hemispheres of the *** findings indicate that the white light polarization is lower in the lunar highland than in the lunar maria *** the analysis of lunar soil samples,we noticed and determined that the DOP parameters of white light demonstrate high consistency with iron oxide on the *** study may serve as a new diagnostic tool for the Moon.

关键词： techniques:photometric polarization methods:observational Moon