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Role of bonding filling on HER/OER/ORR multifunctional catalytic activity in transition-metals-doped PdPX(X=S,Se,Te)

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Rare Metals 2024年第10期43卷 5126-5140页

作者： Hai-Hua Huang Wei Li cheng-Chao Hu Xue-Qin Sun Lin-Guo Lu xiao-Feng Fan School of Materials Science and Engineering Laboratory of Sensitive Materials and DevicesShandong Department of EducationLiaocheng University School of Environmental and Material Engineering Yantai University Department of Physics University of Puerto Rico Key Laboratory of Automobile Materials (Jilin University) Ministry of EducationCollege of Materials Science and EngineeringJilin University

The development of stable and highly efficien multifunctional electrocatalysts for the hydrogen evolution reaction （HER）,oxygen reduction reaction （ORR） and oxygen evolution reaction （OER） are essential for the efficient conversion and storage of renewable *** significant advantages of single-atom catalysts,such as strong metal slab interactions,unsaturated coordination and efficient atomic utilization,have opened new avenues for designing multifunctional ***,based on density functional theory,a single atom doped PdPX system was designed as a multifunctional electrocatalyst,which demonstrated the synergistic effect between defects and transition metal atoms and led to enhanced catalytic *** results showed that PdPS/PdPSe with P/X vacancy,PdPTe with P/Pd vacancy and Co/Rh/Ir@PdPX exhibited promising HER ***@PdPS（Se）,with an overpotential of 0.56（0.44） V,was predicted to be a promising OER ***,Rh（Ir）@PdPS（Se）catalysts exhibited efficient catalytic properties for ORR Besides,Co@PdPS（Se）,Rh（Ir）@PdPSV（S）,Co@PdP-SeV（Se）and Ir@PdPSV（S）-1exihibited multifunctional catalytic performance with moderate ***,the origin of catalytic activity was revealed by using the crystal orbital Hamilton populations *** a strong adsorption system,proper filling of the anti-bonding state can increase the energy of the system,weaken the adsorption strength,and facilitate the desorption of intermediates Conversely,augmenting bonding states can enhance its adsorption *** findings provide theoretica guidance for the design and fabrication of novel multifunctional electrocatalysts in terms of filling of bondingstate.

关键词： Density functional theory Electrocatalyst Two-dimensional PdPX Water splitting

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Adsorption behavior of CO2/H2S mixtures in calcite slit nanopores for CO2 storage:An insight from molecular perspective

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Petroleum Science 2024年第4期21卷 2444-2456页

作者： cheng Qian Zhen-Hua Rui Yue-Liang Liu Kai Du Chen Liu Yang Zhao xiao-Min Ma State Key Laboratory of Petroleum Resources and Engineering China University of Petroleum College of Petroleum Engineering China University of Petroleum College of Carbon Neutrality Future Technology China University of Petroleum College of Petroleum China University of Petroleum-Beijing at Karamay College of Mining Engineering Taiyuan University of Technology

It is acknowledged that injecting CO2into oil reservoirs and saline aquifers for storage is a practical and affordable method for *** CO2produced from industrial exhaust contains impurity gases such as H2S that might impact CO2sequestration due to competitive *** study makes a commendable effort to explore the adsorption behavior of CO2/H2S mixtures in calcite slit *** Canonical Monte Carlo（GCMC） simulation is employed to reveal the adsorption of CO2,H2S as well as their binary mixtures in calcite *** show that the increase in pressure and temperature can promote and inhibit the adsorption capacity of CO2and H2S in calcite nanopores,***2exhibits stronger adsorption on calcite surface than *** energy plays the dominating role in the adsorption *** energy accounts for 97.11% of the CO2-calcite interaction energy and 56.33% of the H2S-calcite interaction energy at 10 MPa and 323.15 *** presence of H2S inhibits the CO2adsorption in calcite nanopores due to competitive adsorption,and a higher mole fraction of H2S leads to less *** quantity of CO2adsorbed is lessened by approximately 33% when the mole fraction of H2S reaches ***2molecules preferentially occupy the regions near the po re wall and H2S molecules tend to reside at the center of nanopore even when the molar ratio of CO2is low,indicating that CO2has an adsorption priority on the calcite surface over *** addition,moisture can weaken the adsorption of both CO2and H2S,while CO2is more *** interestingly,we find that pure CO2is more suitable to be sequestrated in the shallower formations,i.e.,500-1500 m,whereas CO2with H2S impurity should be settled in the deeper reservoirs.

关键词： Adsorption behavior CO2/H2S binary mixtures Molecular perspective Calcite slit nanopores CO2 sequestration

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Stable Cycling of All-Solid-State Lithium Batteries Enabled by Cyano-Molecular Diamond Improved Polymer Electrolytes

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Nano-Micro Letters 2024年第10期16卷 561-575页

作者： Yang Dai Mengbing Zhuang Yi-xiao Deng Yuan Liao Jian Gu Tinglu Song Hao Yan Jin-cheng Zheng Department of Chemical Engineering Shanghai UniversityShangda Road 99Shanghai 200444People's Republic of China Department of Physics Xiamen UniversityXiamen 361005People's Republic of China Experimental Center of Advanced Materials School of Materials Science and Engineering Beijing Institute of TechnologyBeijing 100081People's Republic of China Department of Physics and Department of New Energy Science and Engineering Xiamen University Malaysia43900 SepangMalaysia

The interfacial instability of the poly(ethylene oxide)(PEO)-based electrolytes impedes the long-term cycling and further application of all-solid-state lithium metal *** this work,we have shown an effective additive 1-adaman-tanecarbonitrile,which con-tributes to the excellent per-formance of the poly(ethylene oxide)-based *** to the strong interaction of the 1-Adamantanecarboni-trile to the polymer matrix and anions,the coordination of the Li^(+)-EO is weakened,and the binding effect of anions is strengthened,thereby improving the Li^(+)conductivity and the electrochemical *** diamond building block on the surface of the lithium anode can sup-press the growth of lithium ***,the 1-Adamantanecarbonitrile also regulates the formation of LiF in the solid electrolyte interface and cathode electrolyte interface,which contributes to the interfacial stability(especially at high voltages)and protects the electrodes,enabling all-solid-state batteries to cycle at high voltages for long periods of ***,the Li/Li symmetric cell undergoes long-term lithium plating/stripping for more than 2000 h.1-Adamantanecarbonitrile-poly(ethylene oxide)-based LFP/Li and 4.3 V Ni_(0.8)Mn_(0.1)Co_(0.1)O_(2)/Li all-solid-state batteries achieved stable cycles for 1000 times,with capacity retention rates reaching 85%and 80%,respectively.

关键词： 1-Adamantanecarbonitrile(ADCN) Poly(ethylene oxide) All-solid-state batteries Interfacial stability High voltage

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A compact route for efficient production of high-purity β-Ga_(2)O_(3) powder

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Rare Metals 2024年第9期43卷 4573-4584页

作者： xiao-Wei Zhou Gao-Jie Chen Liang Xu Zhi-Jun Shao cheng Yang Yong-Pan Tian Zhuo Zhao School of Metallurgical Engineering Anhui University of TechnologyMa'anshan 243032China Low-Carbon Research Institute Anhui University of TechnologyMa'anshan 243032China

The present study has proposed a compact process for the production of high-purity β-Ga_(2)O_(3)powder by simply using gallium metal and water as the raw *** process basically consists of two essential steps including hydrothermal synthesis of Ga OOH and calcination of Ga OOH for the production of the target product of β-Ga_(2)O_(3).Thermodynamic evaluation and systematic experiments were conducted for process parameter optimization.X-ray diffractometer(XRD),scanning electron microscopy(SEM),thermogravimetryDdifferential scanning calorimetry(TG-DSC)and X-ray photoelectron spectroscopy(XPS)were utilized to clarify the reaction mechanisms of the hydrothermal synthesis and transformation of Ga OOH to β-Ga_(2)O_(3)by *** analysis of the final product of β-Ga_(2)O_(3)obtained under the optimal conditions was carried out with inductively coupled plasma mass spectrometry(ICP-MS),and the results showed that the contents of the representative impurities such as Ni,Cu,In,Mn,Co,Zn and Cr are obviously lower than the requirement of 5N β-Ga_(2)O_(3)standard,exhibiting excellent application prospect of the proposed process to produce high-purity β-Ga_(2)O_(3).

关键词： β-Ga_(2)O_(3) Hydrothermal synthesis Calcination Purity Reaction mechanism

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Quantification of Central and Eastern China's atmospheric CH_(4) enhancement changes and its contributions based on machine learning approach

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Journal of Environmental Sciences 2024年第4期138卷 236-248页

作者： Xinyue Ai cheng Hu Yanrong Yang Leying Zhang Huili Liu Junqing Zhang Xin Chen Guoqiang Bai Wei xiao College of Biology and the Environment Joint Center for sustainable Forestry in Southern ChinaNanjing Forestry UniversityNanjing 210037China Collaborative Innovation Center on Forecast and Evaluation of Meteorological Disasters(CIC-FEMD) Nanjing University of Information Science&TechnologyNanjing 210044China Guang’an Vocational&Technical College Guangan 638550China HuaNan Meteorological Administration Huanan 154400China

Methane is the second largest anthropogenic greenhouse gas,and changes in atmospheric methane concentrations can reflect the dynamic balance between its emissions and ***,the monitoring of CH_(4) concentration changes and the assessment of underlying driving factors can provide scientific basis for the government’s policy making and *** is the world’s largest emitter of anthropogenic ***,due to the lack of ground-based observation sites,little work has been done on the spatial-temporal variations for the past decades and influencing factors in China,especially for areas with high anthropogenic emissions as Central and Eastern *** to quantify atmospheric CH_(4) enhancements trends and its driving factors in Central and Eastern China,we combined the most up-to-date TROPOMI satellite-based column CH_(4)(xCH_(4))concentration from 2018 to 2022,anthropogenic and natural emissions,and a random forest-based machine learning approach,to simulate atmospheric xCH_(4) enhancements from 2001 to *** results showed that(1)the random forest model was able to accurately establish the relationship between emission sources and xCH_(4) enhancement with a correlation coefficient(R^(2))of 0.89 and a root mean-square error(RMSE)of 11.98 ppb;(2)The xCH_(4) enhancement only increased from 48.21±2.02 ppb to 49.79±1.87 ppb from the year of 2001 to 2018,with a relative change of 3.27%±0.13%;(3)The simulation results showed that the energy activities and waste treatment were the main contributors to the increase in xCH_(4) enhancement,contributing 68.00% and 31.21%,respectively,and the decrease of animal ruminants contributed-6.70% of its enhancement trend.

关键词： TROPOMI Methane column concentrations Anthropogenic sources Random Forest model

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Matrix metalloproteinase 2 degrades collagen I to regulate ovarian development by association with an insulin-like peptide

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Insect Science 2024年第4期31卷 1090-1106页

作者： Yi Wei xiao-Lin Zhou Peng Chen Tai-Hang Liu cheng Lu Min-Hui Pan State Key Laboratory of Silkworm Genome Biology Southwest UniversityChongqingChina Key Laboratory for Sericulture Functional Genomics and Biotechnology of Agricultural Ministry Southwest UniversityChongqingChina Wenzhou Institute University of Chinese Academy of SciencesWenzhouZhejiang ProvinceChina

The ovary generally undergoes tissue remodeling during larval to pupal transition,which includes membrane degeneration and ovariole *** the same time,the hormones produced by insects significantly change during ***,the regulatory mechanism for ovarian development and hormones is not fully understood in ***,we found that matrix metalloproteinase 2(MMP2)was highly expressed in the ovarian capsules and ovarioles,and the development was abnormal after knocking out MMP2 in Bombyx *** process of abnormal degradation of collagen I due to MMP2 deletion,which resulted in abnormal development of ovarioles and eggs,was analyzed in *** proteomics of ovaries in the MMP2-knock out and wild type strains showed a critically significant difference in the expression of a protein,insulin-like peptide(ILP).Additional analysis revealed significant alteration of ILP during ovarian development,and abnormal expression of ILP significantly affected ovarian development in vivo and MMP2 expression in vitro and in *** results showed that MMP2 regulation of ovarian tissue remodeling is closely related to ILP *** study provides new insights into the regulatory mechanism of MMP2 and ovarian development in ***.

关键词： Bombyx mori collagen I insulin-like peptide matrix metalloproteinase ovarian development

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Switchable Multicomponent Cyclization Reactions to Access Fluoroalkylated Dihydropyrimidines and Pyrimidines under Solvent-Free Conditions

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Chinese Journal of Chemistry 2024年第12期42卷 1394-1398页

作者： Wanqing Zuo Zhizhen Zhu Yu cheng Lingling Zuo xiao Geng Zhifang Li Lei Wang College of Material Chemistry and Chemical Engineering Key Laboratory of Organosilicon Chemistry and Material TechnologyMinistryof EducationHangzhouNormal UniversityHangzhouZhejiang311121China Advanced Research Institute and School of Pharmaceutical Sciences Taizhou UniversityJiaojiangZhejiang 318000China state Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai200032China

Comprehensive Summary The development of switchable solvent-free multicomponent reactions to build high-value-added products is an important demand for organic ***,we detailed the successful implementation of a switchable strategy for the construction of diverse 4-fluoroalkyl-1,4-dihydropyrimidines and 4-fluoroalkyl-pyrimidines via a solvent/additive-free[3+2+1]annulation,starting from readily available enamines,trifluoroacetaldehyde hydrate or 1-ethoxy-2,2-difluoroethanol and amidines *** reaction conforms to the concept of green synthesis,and provides a new avenue to access valuable fluorinated heterocycles.

关键词： Fluorine chemistry Multicomponent reactions Environmental chemistry Heterocycles Enaminones Amidines

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Genetic analysis and fine mapping of a grain size QTL in the smallgrain sterile rice line Zhuo201S

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Journal of Integrative Agriculture 2024年第7期23卷 2155-2163页

作者： Bin Lei Jiale Shao Feng Zhang Jian Wang Yunhua xiao Zhijun cheng Wenbang Tang Jianmin Wan College of Agronomy Hunan Agricultural UniversityChangsha 410128China National Key Facility for Crop Gene Resources and Genetic Improvement/Institute of Crop Sciences Chinese Academy of Agricultural SciencesBeijing 100081China State Key Laboratory for Crop Genetics and Germplasm Enhancement/Jiangsu Plant Gene Engineering Research Center Nanjing Agricultural UniversityNanjing 210095China State Key Laboratory of Hybrid Rice Hunan Hybrid Rice Research CenterChangsha 410125China

The development and application of the small-grain rice sterile line Zhuo201S(Z201S)has demonstrated its potential for mechanized hybrid rice seed production,leading to significant cost ***,the molecular mechanism responsible for the small-grain size characteristic of Z201S remains *** this study,we conducted a genetic analysis using near-isogenic lines constructed from Z210S,a small-grain rice sterile line,and R2115,a normal-grain *** results revealed that the small-grain trait in Z201S is governed by a single partially dominant gene which also enhances grain *** mapping,we localized the causal gene to the short arm of chromosome 2,within a 113 kb physical region delimited by the molecular markers S2-4-1 and *** analysis and gene expression assays indicated LOC_Os02g14760 as the most likely candidate gene,suggesting that the small-grain size trait of Z201S is controlled by a novel locus that has not been previously identified.

关键词： rice grain size map-based cloning

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A near-infrared fluorescent probe for visualizing transformation pathway of Cys/Hcy and H2S and its applications in living system

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Chinese Chemical Letters 2024年第5期35卷 296-301页

作者： Yudi cheng xiao Wang Jiao Chen Zihan Zhang Jiadong Ou Mengyao She Fulin Chen Jianli Li Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education Xi’an Key Laboratory of Functional Supramolecular Structure and MaterialsCollege of Chemistry&Materials ScienceNorthwest UniversityXi’an 710127China Key Laboratory of Resource Biology and Biotechnology in Western China Ministry of EducationBiomedicine Key Laboratory of Shaanxi ProvinceLab of Tissue Engineeringthe College of Life SciencesFaculty of Life Science&MedicineNorthwest UniversityXi’an 710069China

Sulfydryl-contained(-SH)substances including hydrogen sulfide(H_(2)S),cysteine(Cys),homocysteine(Hcy)and glutathione(GSH)play crucial roles in living systems,and their variations are closely associated with various ***,we developed a near-infrared intramolecular charge transfer(ICT)based fluorescent probe Y-NBD,achieving detection of Cys/Hcy and H_(2)S with different fluorescent signals(green-red for Cys/Hcy,red for H_(2)S),large Stokes shifts(∼100/105nm or 191 nm)and high signal-background-ratio,but not responding to GSH.Y-NBD was successfully applied to image exogenous/endogenous Cys/Hcy and H_(2)S in various living cancer cells(HeLa,A549,and HepG2)and in *** not only visualized the transformation pathway of several thiols in HepG2 cells but also verified that the intestine is the main site for the activation and metabolism of Y-NBD in zebrafish,as well as realized to evaluate the degree of drug-induced liver *** work provides a promising tool for imaging Cys/Hcy and H_(2)S in living systems and shows great potency in evaluating drug-induced liver injury and its treatment.

关键词： Fluorescent probe Near-infrared Hydrogen sulfide Cysteine/homocysteine Large Stokes shift Dicyanoisophorone Drug-induced liver injury

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Thermo-hydro-poro-mechanical responses of a reservoir-induced landslide tracked by high-resolution fiber optic sensing nerves

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Journal of Rock Mechanics and Geotechnical Engineering 2024年第3期16卷 1018-1032页

作者： xiao Ye Hong-Hu Zhu Gang cheng Hua-Fu Pei Bin Shi Luca Schenato Alessandro Pasuto School of Earth Sciences and Engineering Nanjing UniversityNanjing210023China School of Computer Science North China Institute of Science and Technology(National Safety Training Center of Coal Mines)Beijing101601China State Key Lab of Coastal and Offshore Engineering Department of Geotechnical EngineeringDalian University of TechnologyDalian116024China National Research Council-Research Institute for Geo-Hydrological Protection(CNR-IRPI) Padova35127Italy Department of Information Engineering University of PadovaPadova35131Italy

Thermo-poro-mechanical responses along sliding zone/surface have been extensively ***,it has not been recognized that the potential contribution of other crucial engineering geological interfaces beyond the slip surface to progressive ***,we aim to investigate the subsurface multiphysics of reservoir landslides under two extreme hydrologic conditions(*** and dry),particularly within sliding *** on ultra-weak fiber Bragg grating(UWFBG)technology,we employ specialpurpose fiber optic sensing cables that can be implanted into boreholes as“nerves of the Earth”to collect data on soil temperature,water content,pore water pressure,and *** Xinpu landslide in the middle reach of the Three Gorges Reservoir Area in China was selected as a case study to establish a paradigm for in situ thermo-hydro-poro-mechanical *** UWFBG-based sensing cables were vertically buried in a 31 m-deep borehole at the foot of the landslide,with a resolution of 1 m except for the pressure *** reported field measurements covering the period 2021 and 2022 and produced the spatiotemporal profiles throughout the *** show that wet years are more likely to motivate landslide motions than dry *** annual thermally active layer of the landslide has a critical depth of roughly 9 m and might move downward in warmer *** dynamic groundwater table is located at depths of 9e15 m,where the peaked strain undergoes a periodical response of leap and withdrawal to annual hydrometeorological *** interface behaviors may support the interpretation of the contribution of reservoir regulation to slope stability,allowing us to correlate them to local damage events and potential global *** paper also offers a natural framework for interpreting thermo-hydro-poro-mechanical signatures from creeping reservoir bank slopes,which may form the basis for a landslide monitoring and early warning system.

关键词： Reservoir landslide Thermo-hydro-poro-mechanical response Ultra-weak fiber bragg grating(UWFBG) subsurface evolution Engineering geological interface Geotechnical monitoring

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