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Enhancing Green Ammonia Electrosynthesis Through Tuning Sn Vacancies in Sn‑Based MXene/ MAX Hybrids

Nano-Micro Letters 2024年第5期16卷 154-168页

作者： Xinyu Dai zhen‑Yi Du Ying Sun Ping Chen Xiaoguang Duan Junjun Zhang Hui Li Yang Fu Baohua Jia Lei Zhang Wenhui fang Jieshan Qiu Tianyi Ma Key Laboratory for Green Synthesis and Preparative Chemistry of Advanced Materials of Liaoning Province College of ChemistryInstitute of Clean Energy ChemistryLiaoning UniversityShenyang 110036People’s Republic of China State Key Laboratory of Clean and Efficient Coal Utilization Taiyuan University of TechnologyTaiyuan 030024People’s Republic of China School of Chemistry and Chemical Engineering Anhui UniversityHefei 230601People’s Republic of China School of Chemical Engineering The University of AdelaideAdelaideSA 5005Australia State Key Laboratory of High‑Efficiency Utilization of Coal and Green Chemical Engineering College of Chemistry and Chemical EngineeringNingxia UniversityYinchuan 750021NingxiaPeople’s Republic of China School of Science RMIT UniversityMelbourneVIC 3000Australia Guangdong Provincial Key Laboratory of Advanced Energy Storage Materials School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640People’s Republic of China College of Chemical Engineering State Key Laboratory of Chemical Resource EngineeringBeijing University of Chemical TechnologyBeijing 100029People’s Republic of China

Renewable energy driven N_(2) electroreduction with air as nitrogen source holds great promise for realizing scalable green ammonia production.However,relevant out-lab research is still in its infancy.Herein,a novel Sn-based MXene/MAX hybrid with abundant Sn vacancies,Sn@Ti_(2)CTX/Ti_(2)SnC–V,was synthesized by controlled etching Sn@Ti_(2)SnC MAX phase and demonstrated as an efficient electrocatalyst for electrocatalytic N2 reduction.Due to the synergistic effect of MXene/MAX heterostructure,the existence of Sn vacancies and the highly dispersed Sn active sites,the obtained Sn@Ti2CTX/Ti_(2)SnC–V exhibits an optimal NH_(3) yield of 28.4μg h^(−1) mg_(cat)^(−1) with an excellent FE of 15.57% at−0.4 V versus reversible hydrogen electrode in 0.1 M Na_(2)SO_(4),as well as an ultra-long durability.Noticeably,this catalyst represents a satisfactory NH3 yield rate of 10.53μg h^(−1) mg^(−1) in the home-made simulation device,where commercial electrochemical photovoltaic cell was employed as power source,air and ultrapure water as feed stock.The as-proposed strategy represents great potential toward ammonia production in terms of financial cost according to the systematic technical economic analysis.This work is of significance for large-scale green ammonia production.

关键词： Green ammonia synthesis N2 electroreduction Renewable energy Sn MXene/MAX hybrid

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A chromosome-level genome assembly for Chinese plum‘Wushancuili'reveals the molecular basis of its fruit color and susceptibility to rain-cracking

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Horticultural Plant Journal 2024年第3期10卷 672-688页

作者： Kun zhou Jingwen Wang Lin Pan fang Xiang Yi zhou Wei Xiong Ming Zeng Donald Grierson Wenbin Kong Lingyu Hu Wanpeng Xi College of Horticulture and Landscape Architecture Southwest UniversityChongqing 400715China Key Laboratory of Agricultural Biosafety and Green Production of Upper Yangtze River(Ministry of Education) Southwest UniversityChongqing 400715China Department of Pomology Chongqing Agricultural Technology Extension StationChongqing 401420China Plant and Crop Sciences Division School of BiosciencesUniversity of NottinghamSutton Bonington CampusLoughborough LE125RDUK Wuxi Economical Crop Technology Extension Station Chongqing 405800China

Chinese plum(Prunus salicina Lindl.)originates from China and makes a large contribution to the global production of plums.The P.salicina‘Wushancuili'has a green coloration and high fruit quality and is economically important in eliminating poverty and protecting ecology in the Yangtze River Three Gorges Reservoir.However,rain-induced cracking(rain-cracking,literally skin cracking caused by rain)is a limitation to‘Wushancuili'fruit production and causes severe losses.This study reported a high-quality‘Wushancuili'genome assembly consisting of a 302.17-Mb sequence with eight pseudo-chromosomes and a contig N50 of 23.59 Mb through the combination of Illumina sequencing,Pacific Biosciences HiFiⅢsequencing,and high-throughput chromosome conformation capture technology.A total of 25109 protein-coding genes are predicted and 54.17%of the genome is composed of repetitive sequences.‘Wushancuili'underwent a remarkable orthoselection during evolution.Gene identification revealed that loss-of-function in four core MYB10 genes results in the anthocyanin deficiency and absence of red color,revealing the green coloration due to the residual high chlorophyll in fruit skin.Besides,the occurrence of cracking is assumed to be closely associated with cell wall modification and frequently rain-induced pathogen enrichment through transcriptomic analysis.The loss of MYB10 genes might render fruit more susceptible to pathogen-mediated cracking by weakening the epidermal strength and reactive oxygen species(ROS)scavenging.Our findings provided fundamental knowledge regarding fruit coloration and rain-cracking and will facilitate genetic improvement and cultivation management in Chinese plums.

关键词： Chinese plum Fruit coloration Fruit epidermis Genome MYB10 Rain-cracking

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Dynamically lithium-compensated polymer artificial SEI to assist highly stable lithium-rich manganese-based anode-free lithium metal batteries

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Rare Metals 2024年第6期43卷 2527-2535页

作者： Ming-Ji Peng Jin-Qiu zhou Ting-Ting Han Yang zhou Jie Liu Na Xu zhen-Kang Wang Wen-Bin Lin Cheng-Lin Yan Key Laboratory of Core Technology of High Specific Energy Battery and Key Materials for Petroleum and Chemical Industry College of EnergySoochow University Light Industry Institute of Electrochemical Power Sources School of Chemistry and Chemical Engineering Nantong University State Key Laboratory of Space Power-Sources Technology Shanghai Institute of Space Power-Sources Centre énergie Matériaux et TélécommunicationsInstitut National de la Recherche Scientifique Zhangjiagang Industrial Technologies Soochow University

Owing to the unique structure,anode-free lithium metal batteries（AFLMBs） have higher energy density and lower production cost than traditional lithium metal batteries（LMBs） or lithium-ion batteries（LIBs）,However,AFLMBs suffer from an inherently finite Li reservoir and exhibit poor cycle stability,low Coulombic efficiency（CE） and severe dendrite growth.In this work,polydiallyl lithium disulfide（PDS-Li） was successfully synthesized and coated on Cu current collector by electrochemical polymerization.The PDS-Li acts as an additional lithium resource to compensate for the irreversible loss of lithium during cycling.In addition,the special structure and lithiophilicity of PDS-Li contribute to lower nucleation overpotential and uniform lithium deposition.When coupled with Li-rich manganese-based（LRM）cathode of Li1.2Mn0.54Ni0.13Co0.13O2,the anode-free full cell exhibits significantly improved cycle stability over 100 cycles and capacity retention of 63.3% and 57% after 80 and 100 cycles,respectively.We believe that PDS-Li can be used to ensure stable cycling performance and high-energy-density in AFLMBs.

关键词： Anode-free Artificial solid electrolyte interphase (SEI) Lithium metal batteries Lithium-rich cathode Finite element simulation

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Single thiolate replacement of metal nanoclusters

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Science China Chemistry 2024年第2期67卷 523-528页

作者： Ambreen Ambreen Yue zhou Wanmiao Gu Qing You Liang fang Guoqing Bian Nan Yan Nan Xia Zhikun Wu Key Laboratory of Materials Physics Anhui Key Laboratory of Nanomaterials and NanotechnologyInstitute of Solid State PhysicsHefei Institutes of Physical Science(HFIPS)Chinese Academy of SciencesHefei230031China University of Science and Technology of China Hefei230601China Institute of Physical Science and Information Technology Anhui UniversityHefei230601China

Surface thiolates play important roles in evincing the structures and properties of thiolated metal nanoclusters—one type of recently emerging inorganic-organic hybrids,and thus the thiolate substitution,especially single thiolate substitution,is highly desirable for subtly tailoring the structures and properties of metal nanoclusters.However,such a single-thiolate substituting is challenging,and its influence on the metal-metal and metal-sulfur bonds remains mysterious due to the absence of the singlethiolate-substituted structure.Here,we developed a combined method,concurrently synthesized the single-thiolate-substituted nanocluster and its parent nanocluster,and successfully resolved their structures by single crystal X-ray crystallography,which reveals that the single thiolate substitute has an obvious influence on the metal-metal and metal-sulfur bond lengths although it has no effect on the absorption profile.Interestingly,the metal-metal and metal-sulfur bonds show various thermal extensibility and even the negative thermal expansion phenomena of the Au–S bond were observed in the single-thiolate-substituted nanocluster.The bond length-related stability was also observed.Overall,this study highlights a novel synthesis method and offers novel structural insights and an in-depth structure-property correlation of thiolated metal nanoclusters.

关键词： metal nanoclusters single thiolate replacement thermal expansion stability intercluster interaction

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QL1706 (anti-PD-1 IgG4/CTLA-4 antibody) plus chemotherapy with or without bevacizumab in advanced non-small cell lung cancer: a multi-cohort, phase II study

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Signal Transduction and Targeted Therapy 2024年第2期9卷 797-806页

作者： Yan Huang Yunpeng Yang Yuanyuan Zhao Hongyun Zhao Ningning zhou Yaxiong Zhang Likun Chen Ting zhou Gang Chen Ting Wu Lu Lu Shilin Xue Xiaoyan Kang Li Zhang Wenfeng fang Department of Medical Oncology Sun Yat-sen University Cancer CenterState Key Laboratory of Oncology in South ChinaCollaborative Innovation Center for Cancer MedicineNo.651 Dongfeng East RoadGuangzhouGuangdong 510060China Department of Medicine Qilu Pharmaceutical Co.Ltd.JinanChina

First-line chemoimmunotherapy(with or without bevacizumab)has improved outcomes in advanced non-small cell lung cancer(NSCLC).Here,this open-label,multi-cohort phase II study(NCT05329025)was done to investigate the safety and efficacy of QL1706(a single bifunctional MabPair product against PD-1 and CTLA-4)and chemotherapy with or without bevacizumab in this population.Patients were enrolled into five different cohorts based on genotype(cohorts 1-4,epidermal growth factor receptor[EGFR]wild-type;cohort 5,EGFR-mutant and progressed on EGFR-tyrosine kinase inhibitors[TKIs]).Between June 11,2021 and December 29,2021,91 patients were enrolled.Most frequent treatment-related adverse events(TRAEs)included decreased appetite(60[65.9%]),anemia(60[65.9%]),infusion-related reactions(48[52.7%]),and pruritus(44[48.4%]).Grade≥3 TRAEs occurred in 30(33.0%)patients.Twenty-seven(45%)patients with wild-type EGFR achieved partial response(PR)(objective response rate[ORR]=45%)and had a median progression-free survival(mPFS)of 6.8 months(95%CI:5.2-9.7).For 31 patients harboring mutated EGFR,17(54.8%)achieved PR(ORR=54.8%),with an mPFS of 8.5 months(95%CI:5.72-not evaluable).Overall,QL1706 plus chemotherapy,regardless of having bevacizumab,was generally tolerable and had promising antitumor activity for EGFR wild-type advanced NSCLC in first-line setting.Moreover,QL1706 plus chemotherapy and bevacizumab showed favorable antitumor activity for patients who had EGFR mutated NSCLC but failed in TKI therapy,demonstrating a potential for treating this population.

关键词： bevacizumab chemotherapy phase

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Low-noise and low-power pixel sensor chip for gas pixel detectors

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Nuclear Science and Techniques 2024年第3期35卷 142-152页

作者： Zhuo zhou Shi-Qiang zhou Dong Wang Xiang-Ming Sun Chao-Song Gao Peng-zhen Zhu Wei-Ping Ren Jun Liu Mu-Xian Li Chen Lian Chun-Lai Dong PLAC Key Laboratory of Quark and Lepton Physics(MOE)Central China Normal UniversityWuhan 430079China

Topmetal-M2 is a large-area pixel sensor chip fabricated using the GSMC 130 nm CMOS process in 2021.The pixel array of Topmetal-M2 consists of pixels of 400 rows×512 columns with a pixel pitch of 45μm×45μm.The array is divided into 16 subarrays,with pixels of 400 rows×32 columns per subarray.Each pixel incorporates two charge sensors:a diode sensor and a Topmetal sensor.The in-pixel circuit primarily consists of a charge-sensitive amplifier for energy measurements,a discriminator with a peak-holding circuit,and a time-to-amplitude converter for time-of-arrival measurements.The pixel of Topmetal-M2 has a charge input range of~0-3 k e-,a voltage output range of~0-180 mV,and a charge-voltage conversion gain of~59.56μV∕e-.The average equivalent noise charge of Topmetal-M2,which includes the readout electronic system noise,is~43.45 e-.In the scanning mode,the time resolution of Topmetal-M2 is 1 LSB=1.25μs,and the precision is^()7.41μs.At an operating voltage of 1.5 V,Topmetal-M2 has a power consumption of~49 mW∕cm~2.In this article,we provide a comprehensive overview of the chip architecture,pixel working principles,and functional behavior of Topmetal-M2.Furthermore,we present the results of preliminary tests conducted on Topmetal-M2,namely,alpha-particle and soft X-ray tests.

关键词： Charge collection Gas detectors Semiconductor detectors X-ray detectors

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Growth,optical dispersion and magnetic behavior of Dy^(3+) doped yttrium iron garnet crystals

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Journal of Rare Earths 2024年第6期42卷 1110-1117,I0004页

作者： Yating fang Hui Shen Yudie Ma Shijie Liao Shuang Xia Tian Tian Ding zhou Yunfeng Ma Jiayue Xu Institute of Crystal Growth School of Materials Science and EngineeringShanghai Institute of Technology National Engineering Center of Electromagnetic Radiation Control Materials School of Electronic Science and EngineeringUniversity of Electronic Science and Technology of China

Y_(3)Fe_(5)O_(12)(YIG)crystals are highly desirable for the fabrication of mid-infrared isolators with the rapid growth of optical communications,although it is rather challenging to grow large size and high-quality single crystals.Dy^(3+)doping is expected to improve the optical and magneto-optical prope rties.However,high quality Dy:YIG crystals and the adjustment of Dy^(3+)on the structure and optical behavior of YIG crystal remain unclear,impeding its practical applications.Herein,a series of Y_(3-x)Dy_(x)Fe_(5)O_(12)(x=0,0.5,1.0,1.5,3)solid solution crystals was grown by the flux-Bridgman method and single crystals up to 25 mm were obtained.With the introduction of Dy^(3+),lattice parameters are gradually enlarged from 1.2379 nm(YIG)to 1.2420 nm(DyIG).Typical Dy^(3+)absorption peaks are observed around 1070,1265 and 1670 nm.The refractive index decreases from 2.37(500 nm)to 2.10(2500 nm)for YIG crystal,and it reduces from 2.47(500 nm)to 2.16(2500 nm)for DyIG crystal.The optical bandgaps remain almost unchanged for Dy:YIG crystals.The optical dispersion of the refractive indices was finely fitted by the Wemple and DiDomenico(WDD)and the Sellmeier models,respectively.With the increase of Dy^(3+)content,the saturation magnetization(Ms)decreases significantly from 23.62 emu/g(YIG)to 5.33 emu/g(DyIG).Small coercive field is persisted for this system,endowing small external magnetic field.These results provide valuable references for the manipulation of rare earths on the properties of magnetooptical crystals,which is beneficial to the design of high-performance garnet crystals for the application of optical switching and non-reciprocal related devices.

关键词： Magneto-optical crystal Yttrium iron garnet Dy^(3+)doping Crystal growth Optical dispersion Rare earths

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N-doped hollow carbon nanospheres embedded in N-doped graphene forming a three-dimensional interconnected layered porous support loaded with palladium nanoparticles as an efficient electrocatalyst for formic acid oxidation

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新型炭材料(中英文) 2024年

作者： fang Yue YANG Fu-kai QU Wei-li DENG Chao WANG zhen-bo Key Laboratory of Photochemical Biomaterials and Energy Storage Materials Shenzhen Key Laboratory of Special Functional Materials Shenzhen Engineering Laboratory for Advance Technology of Ceramics Guangdong Research Center for Interfacial Engineering of Functional Materials College of Materials Science and Engineering Shenzhen University MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering State Key Lab of Urban Water Resource and Environment Harbin Institute of Technology College of Chemistry and Chemical Engineering Harbin Normal University No.1 Normal University South Road

The efficient electrocatalysts with low cost, high activity and good durability plays a crucial role in the application of direct formic acid fuel cells. Herein, Pd nanoparticles supported on N-doped hollow carbon nanospheres (NHCN) embedded in Ndoped graphene (NG) with three-dimensional (3D) layered porous configuration by a simple and economical method were investigated as direct formic acid fuel cell catalysts. Owing to the unique 3D interconnected layered porous configuration doped with nitrogen atoms, Pd/NHCN@NG catalyst with smaller Pd nanoparticle size shows large catalytic active surface area, superior electrocatalyticactivity,highsteady-statecurrentdensity,strongabilitytoresistCOpoisoning,farsurpassingthoseofconventionalPd/C,Pd/NG,andPd/***/GOratio,itisfoundthatwhenthe HCN/GO mass ratio is 1∶1, Pd/NHCN@NG catalyst has the most outstanding performance in catalytic oxidation of formic acid,with an activity 4.21 times that of Pd/C. This work has developed a superior carbon-based support material for electrocatalysts, which brings broad application prospects for the development of fuel cells.

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Reynosin protects neuronal cells from microglial neuroinflammation by suppressing NLRP3 inflammasome activation mediated by NADPH oxidase

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Chinese Journal of Natural Medicines 2024年第6期22卷 486-500页

作者： YANG Yanqiu CHE Yue fang Mingxia YAO Xiaohu zhou Di WANG Feng CHEN Gang LIANG Dong LI Ning HOU Yue Key Laboratory of Bioresource Research and Development of Liaoning Province College of Life and Health SciencesNorth-eastern UniversityShenyang 110000China National Frontiers Science Center for Industrial Intelligence and Systems Optimization Key Laboratory of Data Analytics and Optimization for Smart IndustryMinistry of EducationNortheastern UniversityShenyang 110000China School of Traditional Chinese Materia Medica Key Laboratory of Innovative Traditional Chinese Medicine for Major Chronic Diseases of Liaoning provinceKey Laboratory for TCM Material Basis Study and Innovative Drug Development of Shenyang CityShenyang Pharmaceutical UniversityShenyang 110000China State Key Laboratory for Chemistry and Molecular Engineering of Medicinal Resources School of Chemistry and Pharmaceutical SciencesGuangxi Normal UniversityGuilin 541000China

Neuroinflammation,mediated by the nucleotide-binding oligomerization domain-like receptor family pyrin domain-containing-3(NLRP3)inflammasome,is a significant contributor to the pathogenesis of neurodegenerative diseases(NDDs).Reynos-in,a natural sesquiterpene lactone(SL),exhibits a broad spectrum of pharmacological effects,suggesting its potential therapeutic value.However,the effects and mechanism of reynosin on neuroinflammation remain elusive.The current study explores the effects and mechanisms of reynosin on neuroinflammation using mice and BV-2 microglial cells treated with lipopolysaccharide(LPS).Our findings reveal that reynosin effectively reduces microglial inflammation in vitro,as demonstrated by decreased CD11b expression and lowered interleukin-1 beta(IL-1β)and interleukin-18(IL-18)mRNA and protein levels.Correspondingly,in vivo,results showed a re-duction in the number of Iba-1 positive cells and alleviation of morphological alterations,alongside decreased expressions of IL-1βand IL-18.Further analysis indicates that reynosin inhibits NLRP3 inflammasome activation,evidenced by reduced transcription of NLRP3 and caspase-1,diminished NLRP3 protein expression,inhibited apoptosis-associated speck-like protein containing a CARD(ASC)oli-gomerization,and decreased caspase-1 self-cleavage.Additionally,reynosin curtailed the activation of nicotinamide adenine dinuc-leotide phosphate(NADPH)oxidase,demonstrated by reduced NADP^(+)and NADPH levels,downregulation of gp91^(phox) mRNA,pro-tein expression,suppression of p47^(phox) expression and translocation to the membrane.Moreover,reynosin exhibited a neuroprotective effect against microglial inflammation in vivo and in vitro.These collective findings underscore reynosin’s capacity to mitigate mi-croglial inflammation by inhibiting the NLRP3 inflammasome,thus highlighting its potential as a therapeutic agent for managing neuroinflammation.

关键词： Microglia NLRP3 inflammasome Reactive oxygen species NADPH oxidase Neuron Reynosin

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Black-box membership inference attacks based on shadow model

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The Journal of China Universities of Posts and Telecommunications 2024年

作者： Han zhen zhou Wenan Han Xiaoxuan Wu Jie School of Computer Science Beijing University of Posts and Telecommunications

Membership inference attacks on machine learning models have drawn significant attention. While current research primarily utilizes shadow modeling techniques， which require knowledge of the target model and training data， practical scenarios involve black-box access to the target model with no available information. Limited training data further complicates the implementation of these attacks. In this paper， we experimentally compare common data enhancement schemes and propose a data synthesis framework based on the variational autoencoder generative adversarial network (VAE-GAN) to extend the training data for shadow models. Meanwhile， this paper proposes a shadow model training algorithm based on adversarial training to improve the shadow model’ ability to mimic the predicted behavior of the target model when the target model's information is unknown. By conducting attack experiments on different models under the black-box access setting， this paper verifies the effectiveness of the VAE-GAN-based data synthesis framework for improving the accuracy of membership inference attack. Furthermore， we verify that the shadow model， trained using the adversarial training approach， effectively improves the degree of mimicking the predicted behavior of the target model. Compared with existing research methods， the method proposed in this paper achieves a 2% improvement in attack accuracy and delivers better attack performance.

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