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Non-bonding modulations between single atomic cerium and monodispersed selenium sites towards efficient oxygen reduction

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Nano Research 2024年第6期17卷 4753-4763页

作者： Leilei Yin Shuai Zhang Mingzi Sun Siyuan Wang Bolong Huang Yaping Du Tianjin Key Lab for Rare Earth Materials and Applications Center for Rare Earth and Inorganic Functional MaterialsHaihe Laboratory of Sustainable Chemical TransformationsSmart Sensing Interdisciplinary Science CenterSchool of Materials Science and EngineeringNational Institute for Advanced MaterialsNankai UniversityTianjin 300350China department of applied biology and chemical technology The Hong Kong Polytechnic UniversityHung HomKowloon 999077Hong KongChina Research Centre for Carbon-Strategic Catalysis The Hong Kong Polytechnic UniversityHung HomKowloon 999077Hong KongChina

Currently,dual atomic catalysts(DACs)with neighboring active sites for oxygen reduction reaction(ORR)still meet lots of challenges in the synthesis,especially the construction of atomic pairs of elements from different blocks of the periodic ***,a“rare earth(Ce)-metalloid(Se)”non-bonding heteronuclear diatomic electrocatalyst has been constructed for ORR by rational coordination and carbon support defect ***,the optimized Ce-Se diatomic catalysts(Ce-Se DAs/NC)displayed a half-wave potential of 0.886 V *** hydrogen electrode(RHE)and excellent stability,which surpass those of separate Ce or Se single atoms and most single/dual atomic catalysts ever *** addition,a primary zinc-air battery constructed using Ce-Se DAs/NC delivers a higher peak power density(209.2 mW·cm^(−2))and specific capacity(786.4 mAh·gZn^(−1))than state-of-the-art noble metal catalysts Pt/*** calculations reveal that the Ce-Se DAs/NC has improved the electroactivity of the Ce-N_(4)region due to the electron transfer towards the nearby Se specific activity(SA)***,the more electron-rich Se sites promote the adsorptions of key intermediates,which results in the optimal performances of ORR on Ce-Se DAs/*** work provides new perspectives on electronic structure modulations via non-bonded long-range coordination micro-environment engineering in DACs for efficient electrocatalysis.

关键词： catalyst rare earth oxygen reduction reaction(ORR) metalloid non-bonding modulation

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Molecule aging induced by electron attacking

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Journal of Energy Chemistry 2024年第6期93卷 519-525,I0013页

作者： Ping Song Yining Dong Xue Gong Mingbo Ruan Baoxin Ni Xuanhao Mei Kun Jiang Weilin Xu State Key Laboratory of Electroanalytical Chemistry and Jilin Province Key Laboratory of Low Carbon chemical Power Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of applied Chemistry and Engineering University of Science and Technology of Chin1Hefei 230026AnhuiChina Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Collaborative Innovation Center of Chemistry for Energy MaterialsDepartment of ChemistryFudan UniversityShanghai 200438China

Here we propose a new concept of"molecule aging":with some special treatment,a molecule could be"aged"by losing some unknown tiny particles or pieces from atoms in the molecule,Such"aging"or loss of unknown tiny particles does not change apparently its molecular structure or chemical composition,but some physicochemical properties could be changed *** further confirm such"molecule aging"via a long-term electron attacking to age water(H_(2)O)*** IR spectra show no structural difference between the fresh water and the aged one,while the NMR spectra show that the electron attacking can decrease the size of water *** facts indicate that the electron attacking indeed can"affect"the structure of water molecule slightly but without damaging to its basic molecule *** exploration reveals that the hydrogen evolution reaction(HER)activity of the aged water molecule is lower than the fresh water on the same Pt/C *** density functional theory calculations indicate that the shortened O-H bond in H_(2)O indeed can present lower HER activity,so the observed size decrease of water clusters from NMR probably could be attributed to the shortening of O-H bond in water *** results indicate significantly that the molecule aging can produce materials with new functions for new possible applications.

关键词： Aging of molecules Electron attacking Full width at half maxima Hydrogen evolution reaction

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Differentially-grown cobalt regulators cooperatively involved in the tandem catalysis for high-yield production of second amines

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Nano Research 2024年第4期17卷 2444-2450页

作者： Jinhui Xu Xiao Wang Ying Wang Fei Wang Lingling Zhang Wenjie Cui Shuyan Song Hongjie Zhang State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026China department of Chemistry Tsinghua UniversityBeijing 100084China

One-pot tandem catalysis has been regarded as one of the most atomic economic ways to produce secondary amines,the important platform molecules for chemical synthesis and pharmaceutical manufacture,but it is facing serious issues in overall *** promotional effects are highly desired for boosting the activity and regulating the selectivity of conventional tandem *** this work,we report a high-performance tandem catalyst with maximized synergistic effect among each counterpart by preciously manipulating the spatial structure,which involves the active CeO_(2)/Pt component as kernel,the densely-coated N-doped C(NC)layer as selectivity controller,and the differentially-grown Co species as catalytic performance *** comprehensive investigations,the unique growth mechanism and the promotion effect of Co regulators are ***,the surface-landed Co clusters(Cocs)are crucial to selectivity by altering the adsorption configuration of benzylideneaniline ***,the inner Co particles(Cops)are essential for activity by denoting their electrons to neighboring *** from the unique promotion effect,a remarkably-improved catalytic efficiency(100%nitrobenzene conversion with 94%N-benzylaniline selectivity)is achieved at a relatively low temperature of 80℃,which is much better than that of CeO_(2)/Pt(100%nitrobenzene conversion with 12%N-benzylaniline selectivity)and CeO_(2)/Pt/NC(35%nitrobenzene conversion with 94%benzylideneaniline selectivity).

关键词： tandem catalysis CeO_(2) hierarchical structure heterogeneous catalyst dual-site materials

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Continuous flow pyrolysis of virgin and waste polyolefins:a comparative study,process optimization and product characterization

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Frontiers of chemical Science and Engineering 2024年第6期18卷 133-149页

作者： Ecrin Ekici Güray Yildiz Magdalena Joka Yildiz Monika Kalinowska ErolŞeker Jiawei Wang Karlsruhe Institute of technology Institute of Catalysis Research and TechnologyEggenstein-Leopoldshafen 76344Germany Izmir Institute of technology Faculty of EngineeringDepartment of Energy Systems EngineeringIzmir 35430Türkiye department of Materials Engineering and Production Faculty of Mechanical EngineeringBialystok University of TechnologyBialystok 15-351Poland department of Agricultural and Food Engineering and Environmental Development Institute of Civil Engineering and EnergeticsFaculty of Civil Engineering and Environmental SciencesBialystok University of Technology15-351 BialystokPoland department of Chemistry Biology and BiotechnologyInstitute of Civil Engineering and EnergeticsFaculty of Civil Engineering and Environmental SciencesBialystok University of TechnologyBialystok 15-351Poland Izmir Institute of technology Faculty of EngineeringDepartment of Chemical EngineeringIzmir 35430Türkiye Energy and Bioproducts Research Institute(EBRI) Aston UniversityBirmingham B47ETUnited Kingdom

Under optimal process conditions,pyrolysis of polyolefins can yield ca.90 wt%of liquid product,i.e.,combination of light oil fraction and heavier *** this work,the experimental findings reported in a selected group of publications concerning the non-catalytic pyrolysis of polyolefins were collected,reviewed,and compared with the ones obtained in a continuously operated bench-scale pyrolysis *** process parameters were used for the pyrolysis of waste and virgin counterparts of high-density polyethylene,low-density polyethylene,polypropylene and a defined mixture of those(i.e.,25:25:50 wt%,respectively).To mitigate temperature drops and enhance heat transfer,an increased feed intake is employed to create a hot melt plastic *** 1.5 g·min^(-1) feed intake,1.1 L·min^(-1) nitrogen flow rate,and a moderate pyrolysis temperature of 450℃,the formation of light hydrocarbons was favored,while wax formation was limited for polypropylene-rich *** of virgin plastics yielded more liquid(maximum 73.3 wt%)than that of waste plastics(maximum 66 wt%).Blending polyethylenes with polypropylene favored the production of liquids and increased the formation of gasoline-range *** products were mainly composed of C3 hydrocarbons,and no hydrogen production was detected due to moderate pyrolysis temperature.

关键词： waste plastics polyolefins chemical recycling pyrolysis alternative fuels waste-to-energy

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Generic Interpretable Reaction Condition Predictions with Open Reaction Condition Datasets and Unsupervised Learning of Reaction Center

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Research 2024年第2期2023卷 773-794页

作者： Xiaorui Wang Chang-Yu Hsieh Xiaodan Yin Jike Wang Yuquan Li Yafeng Deng Dejun Jiang Zhenxing Wu Hongyan Du Hongming Chen Yun Li Huanxiang Liu Yuwei Wang Pei Luo Tingjun Hou Xiaojun Yao Dr.Neher's Biophysics Laboratory for lnnovative Drug Discovery State Key Laboratory of Quality Research in Chinese MedicineMacao Institute for Applied Research in Medicine and HealthMacao University of Science and TechnologyMacao999078China innovation Institute for Artificial Intelligence in Medicine of Zhejiang University College of Pharmaceutical SciencesZhejiang UniversityHangzhou310058China Faculty of applied Sciences Macao Polytechnic UniversityMacao999078China College of Chemistry and chemical Engineering Lanzhou UniversityLanzhou730000China Carbon Silicon AI technology Co. LtdHangzhouZhejiang 310018China Center of Chemistry and chemical biology Guangzhou Regenerative Medicine and Health Guangdong LaboratoryGuangzhou 510530China College of Pharmacy Shaanxi University of Chinese MedicineXianyangShaanxi712044China

Effective synthesis planning powered by deep learning(DL)can significantly accelerate the discovery of new drugs and ***,most DL-assisted synthesis planning methods offer either none or very limited capability to recommend suitable reaction conditions(RCs)for their reaction ***,the prediction of RCs with a DL framework is hindered by several factors,including:(a)lack of a standardized dataset for benchmarking,(b)lack of a general prediction model with powerful representation,and(c)lack of *** address these issues,we first created 2 standardized RC datasets covering a broad range of reaction classes and then proposed a powerful and interpretable Transformer-based RC predictor named *** careful design of the model architecture,pretraining method,and training strategy,Parrot improved the overall top-3 prediction accuracy on catalysis,solvents,and other reagents by as much as 13.44%,compared to the best previous model on a newly curated ***,the mean absolute error of the predicted temperatures was reduced by about 4℃.Furthermore,Parrot manifests strong generalization capacity with superior cross-chemical-space prediction *** analysis indicates that Parrot effectively captures crucial chemical information and exhibits a high level of interpretability in the prediction of *** proposed model Parrot exemplifies how modern neural network architecture when appropriately pretrained can be versatile in making reliable,generalizable,and interpretable recommendation for RCs even when the underlying training dataset may still be limited in diversity.

关键词： versatile absolute generalization

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Visible-light-promoted tandem decarboxylation coupling/cyclization of N-aryl glycines with quinoxalinones: Easy access to tetrahydroimidazo [1,5-a]quinoxalin-4(5H)-ones

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Green Synthesis and Catalysis 2024年第1期5卷 31-34页

作者： Zhen Tang Chao Pi Yangjie Wu Xiuling Cui Henan Key Laboratory of chemical biology and Organic Chemistry Key Laboratory of Applied Chemistry of Henan UniversitiesGreen Catalysis CenterCollege of ChemistryZhengzhou UniversityZhengzhou450052China

A visible-light-promoted formal[2+2+1]cyclization of N-aryl glycines with quinoxalin-2(1H)-ones to synthesize tetrahydroimidazo[1,5-a]quinoxalin-4(5H)-ones have been *** protocol features operational simplicity,mild reaction conditions with blue LED light employing Ru(bpy)3Cl2.6H2O as a photoredox catalyst,a combination of O2 from air and Cu(OAc)2 as the oxidant and broad substrate applicability.

关键词： Cyclization Decarboxylation Visible-light-promoted Quinoxalin-2(1H)-ones Mild conditions

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Dynamic tracking of exsolved PdPt alloy/perovskite catalyst for efficient lean methane oxidation

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Chinese chemical Letters 2024年第4期35卷 170-175页

作者： Yanling Yang Zhenfa Ding Huimin Wang Jianhui Li Yanping Zheng Hongquan Guo Li Zhang Bing Yang Qingqing Gu Haifeng Xiong Yifei Sun College of Energy Xiamen UniversityXiamen 361005China School of Environment and Civil Engineering Dongguan University of TechnologyDongguan 523808China department of Chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China CAS Key Laboratory of Science and technology on applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361102China

Supported Pd based catalysts are considered as the efficient candidates for low-carbon alkane oxidation for their outstanding capability to break C-H bond. Whereas, the irreversible deactivation of Pd based catalysts was still frequently observed. Herein, we reinforced the extruded Pd nanoparticles with quantitive Pt to assemble the evenly distributed Pd Pt nanoalloy onto ferrite perovskite(Pd Pt-LCF) matrix with strengthened robustness of metal/oxide support interface. We further co-achieved the enhanced performance, anti-overoxidation as well as resistance of vapor-poisoning in durability measurement. The operando X-ray photoelectron spectroscopy(O-XPS) combined with various morphology characterizations confirms that the accumulation of surface deep-oxidation species of Pd^(4+) is the culprit for fast activity loss in exsolved Pd system, especially at high temperature of 400 ℃. Conversely, it could be completely suppressed by in-situ alloying Pd with equal amount of Pt, which helps maintain the metastable Pd^(2+)/Pd shell and metallic solid-solution core structure. The density function theory(DFT) calculations further buttress that the dissociation of C–H was facilitated on alloy/perovskite interface which is, on the contrary, resistant toward O–H bond cleavage, as compared to Pd/perovskite. Our work suggests that the modification of exsolved metal/oxide catalytic interface could further enrich the toolkit of heterogeneous catalyst design.

关键词： Exsolution PdPt alloy Operando characterization Methane conversion Deep-oxidation

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Bi_(2)WO_(6)/AgInS_(2)S-scheme heterojunction:Efficient photodegradation of organic pollutant and toxicity evaluation

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Journal of Materials Science & technology 2024年第3期170卷 200-211页

作者： Yanyan Zhao Xu Fan Hongxing Zheng Enzhou Liu Jun Fan Xuejun Wang College of biology Pharmacy and Food Engineering Shangluo UniversityShangluo 726000China QinLing-Bashan Mountains Bioresources Comprehensive Development C.I.C. Shaanxi University of TechnologyHanzhong 723001China School of chemical Engineering Northwest UniversityXi’an 710069China

Constructing of heterojunction was identified as a feasible way to improve photocatalytic activity of *** this work,a n-p type Bi_(2)WO_(6)/AgInS_(2)S-scheme heterojunction was successfully prepared for organic pollutants *** Bi_(2)WO_(6)/AgInS_(2)S-scheme heterojunction exhibited much higher pho-tocatalytic activity towards Rhodamine B(92.24%,expose to visible light for 60 min),norfloxacin(81.73%,expose to visible light for 90 min)and levofloxacin(87.46%,expose to visible light for 90 min)than pure Bi_(2)WO_(6)and pure AgInS_(2).Toxicity analysis indicated the low environmental toxicity of Rhodamine B degradation intermediates for Rye seeds and Sudangrass seeds germination and *** study displayed that AgInS_(2)and Bi_(2)WO_(6)work as the primary photocatalyst to form·O_(2)−and ·OH,*** improved photocatalytic activity of the Bi_(2)WO_(6)/AgInS_(2)S-scheme heterojunction was due to the im-proved light response range and intensified carrier separation ***,a S-scheme charge transfer mechanism including multiple charge transfer channels was *** work could provide an effective strategy for organic pollutants degradation in wastewater.

关键词： Photocatalysis S-scheme heterojunction AgInS_(2) Bi_(2)WO_(6) Toxicity experiments

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Low-density lipoprotein receptor-related protein 2(LRP2)is required for lipid export in the midgut of the migratory locust,Locusta migratoria

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Journal of Integrative Agriculture 2024年第5期23卷 1618-1633页

作者： Yiyan Zhao Weimin Liu Xiaoming Zhao Zhitao Yu Hongfang Guo Yang Yang Hans Merzendorfer Kun Yan Zhu Jianzhen Zhang Research Institute of applied biology Shanxi Key Laboratory of Nucleic Acid BiopesticidesShanxi UniversityTaiyuan 030006China College of Life Science Shanxi UniversityTaiyuan 030006China Interfaculty Institute of Cell biology University of TubingenTubingen 72076Germany Institute of biology University of SiegenSiegen 57076Germany department of Entomology Kansas State UniversityManhattanKS 66506USA

Low-density lipoprotein receptor-related protein 2(LRP2)is a multifunctional endocytic receptor expressed in epithelial *** mammals,it acts as an endocytic receptor that mediates the cellular uptake of cholesterol-containing apolipoproteins to maintain lipid ***,little is known about the role of LRP2 in lipid homeostasis in *** the present study,we investigated the function of LRP2 in the migratory locust Locusta migratoria(LmLRP2).The mRNA of LmLRP2 is widely distributed in various tissues,including integument,wing pads,foregut,midgut,hindgut,Malpighian tubules and fat body,and the amounts of LmLRP2 transcripts decreased gradually in the early stages and then increased in the late stages before ecdysis during the nymphal developmental *** immunohistochemistry revealed that the LmLRP2 protein is mainly located in cellular membranes of the midgut and *** RNAi to silence LmLRP2 caused molting defects in nymphs(more than 60%),and the neutral lipid was found to accumulate in the midgut and surface of the integument,but not in the fat body,of dsLmLRP2-treated *** results of a lipidomics analysis showed that the main components of lipids(diglyceride and triglyceride)were significantly increased in the midgut,but decreased in the fat body and ***,the content of total triglyceride was significantly increased in the midgut,but markedly decreased in the fat body and hemolymph in dsLmLRP2-injected *** results indicate that LmLRP2 is located in the cellular membranes of midgut cells,and is required for lipid export from the midgut to the hemolymphand fat body in locusts.

关键词： Locusta migratoria low-density lipoprotein receptor-related protein 2 midgut lipids transport RNAi

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Two sex pheromone receptors for sexual communication in the American cockroach

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Science China(Life Sciences) 2024年第7期67卷 1455-1467页

作者： Na Li Renke Dong Huanchao Zeng Yan Zhang Run Huang Wei Liu Fengming Cao Jincong Yu Mingtao Liao Jingyou Chen Wenlei Zhang Zejian Huang Jiahui Wang Li Li Shen Zhu Danyan Huang Zining Li Xiaoshuai Zhang Dongwei Yuan Nan Chen Yongliang Fan Guirong Wang Coby Schal Yufeng Pan Sheng Li Guangdong Provincial Key Laboratory of Insect Developmental biology and applied technology Institute of Insect Science and TechnologySchool of Life SciencesSouth China Normal UniversityGuangzhou 510631China Guangmeiyuan R&D Center Guangdong Provincial Key Laboratory of Insect Developmental Biology and Applied TechnologySouth China Normal UniversityMeizhou 514589China Lingnan Guangdong Laboratory of Modern Agriculture Genome Analysis Laboratory of the Ministry of AgricultureAgricultural Genomics Institute at ShenzhenChinese Academy of Agricultural SciencesShenzhen 518000China State Key Laboratory of Crop Stress biology for Arid Areas and Key Laboratory of Integrated Pest Management on the Loess Plateau of Ministry of AgricultureNorthwest A&F UniversityYangling 712100China department of Entomology and Plant Pathology North Carolina State UniversityRaleigh 27695USA The Key Laboratory of Developmental Genes and Human Disease School of Life Science and TechnologySoutheast UniversityNanjing 210096China

Volatile sex pheromones are vital for sexual communication between males and *** of the American cockroach,Periplaneta americana,produce and emit two sex pheromone components,periplanone-A(PA)and periplanone-B(PB).Although PB is the major sex attractant and can attract males,how it interacts with PA in regulating sexual behaviors is still *** this study,we found that in male cockroaches,PA counteracted PB *** identified two odorant receptors(ORs),OR53 and OR100,as PB/PA and PA receptors,***53 and OR100 were predominantly expressed in the antennae of sexually mature males,and their expression levels were regulated by the sex differentiation pathway and nutrition-responsive *** localization of OR53 and OR100 in male antennae further revealed that two types of sensilla coordinate a complex two-pheromone-two-receptor pathway in regulating cockroach sexual *** findings indicate distinct functions of the two sex pheromone components,identify their receptors and possible regulatory mechanisms underlying the male-specific and age-dependent sexual behaviors,and can guide novel strategies for pest management.

关键词： sex pheromone odorant receptor sexual attraction sex differentiation cockroach

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