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Asymmetric Zn-N_4 atomic sites embedded hollow fibers as stable Zn anode for high-performance Zn-ion hybrid capacitor
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作者 Yukun Liu Bing Li +5 位作者 Jin Wang Caiyun Li Hongrui Yang Yang Song Sen Zhang Chao Deng 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第10期460-469,I0009,共11页
Zn based electrochemical energy storage systems(EES)have attracted tremendous interests owing to their low cost and high intrinsic safety.Nevertheless,the uncontrolled growth of Zn dendrites and the side reactions of ... Zn based electrochemical energy storage systems(EES)have attracted tremendous interests owing to their low cost and high intrinsic safety.Nevertheless,the uncontrolled growth of Zn dendrites and the side reactions of Zn metal anodes(ZMAs)severely restrict their applications.To address these issues,we design the asymmetric Zn-N_(4) atomic sites embedded hollow fibers(AS-IHF)as the flexible host for stable ZMAs.Through introducing different nitrogen resources in the synthesis,two kinds of coordination,i,e.Zn-N(pyridinic)and Zn-N(pyrrolic),are introduced in the Zn-N_(4) atomic module synchronously.The asymmetric Zn-N_(4) module with regulated micro-environment facilitates the superior zincophilic features and promotes the Zn adsorption.Meanwhile,the highly porous structure of the hollow fiber effectively reduces local current density,homogenize Zn ion flux,and alleviate structure stress.All the advantages endow the high efficiency and good stability for Zn plating/stripping.Both theoretical and experimental results demonstrate the high reversibility,low nucleation overpotential,and dendritefree behavior of the AS-IHF@Zn anode,which afford the high stability in high-rate and long-term cycling.Moreover,the solid-state Zn-ion hybrid capacitor(ZIHC)based on AS-IHF@Zn anode shows the high flexibility,reliability,and superior long-term cycling capability in a wide-range of temperatures(-20-25℃).Therefore,the present work not only gives a new strategy for modulating local environments of single atomic sites,but also propels the development of flexible power sources for diverse electronics. 展开更多
关键词 Asymmetric coordination Single atomic sites Zincophilic sites Dendrite free behavior Zn-ion hybrid capacitor
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d-Orbital steered FeN_(4)moiety through N,S dual-site adjustation for zinc-air flow battery
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作者 Chunzhu Bao Mingwei Tong +1 位作者 Xueli Li Zhonghua Xiang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第5期8-15,共8页
The implementation of pristine covalent organic polymer(CO_(2)P)with well-defined structure as air electrode may spark fresh vitality to rechargeable zinc-air flow batteries(ZAFBs),but it still remains challenges in s... The implementation of pristine covalent organic polymer(CO_(2)P)with well-defined structure as air electrode may spark fresh vitality to rechargeable zinc-air flow batteries(ZAFBs),but it still remains challenges in synergistically regulating their electronic states and structural porosity for the great device performance.Here,we conquer these issues by exploiting N and S co-doped graphene with COP rich in metal-ligand nitrogen to synergistically construct an effective catalyst for oxygen reduction reaction(ORR).Among them,the N and S co-doped sites with high electronegativity properties alter the number of electron occupations in the d orbital of the iron centre and form electron-transfer bridges,thereby boosting the selectivity of the ORR-catalysed four-electron pathway.Meanwhile,the introduction of COP materials aids the formation of pore interstices in the graphene lamellae,which both adequately expose the active sites and facilitate the transport of reactive substances.Benefiting from the synergistic effect,as-prepared catalyst exhibits excellent half-wave potentials(E_(1/2)=912 mV)and stability(merely 8.8%drop after a long-term durability test of 50000 s).Further,ZAFBs assembled with the N/SG@CO_(2)P catalyst demonstrate exceptional power density(163.8 mW cm^(-2))and continuous charge and discharge for approximately 140 h at 10 mA cm^(-2),outperforming the noble-metal benchmarks. 展开更多
关键词 Nitrogen/sulfurdual sites Metal-coordinated nitrogen sites Covalent organic polymer Oxygen reduction reaction Zn-airflow battery
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可持续场地倡议(SITES)评价体系在中国城市绿地建设中的研究进展及适用性讨论
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作者 林广思 朱欣 贺肖淇 《广东园林》 2024年第2期2-6,共5页
建设可持续的城市绿地是风景园林行业实现可持续发展的重要途径。然而,中国目前缺乏指导可持续景观建设的标准体系。可持续场地倡议(SITES)体系的提出和引入为国内相关研究提供了新的切入点。以SITES评价体系为研究对象,概述其起源、主... 建设可持续的城市绿地是风景园林行业实现可持续发展的重要途径。然而,中国目前缺乏指导可持续景观建设的标准体系。可持续场地倡议(SITES)体系的提出和引入为国内相关研究提供了新的切入点。以SITES评价体系为研究对象,概述其起源、主要内容等,明确其在城市绿地项目建设中的应用价值,全面总结了SITES评价体系在国内研究与应用方面的进展,同时深入探讨了其在中国城市绿地建设中的适用性和局限性。SITES在关注“场地”尺度、覆盖全生命周期、设置“门槛”条件以及全球统一标准等方面展现了较强的适用性,然而,在实际应用于中国城市绿地项目时存在一定的局限性,包括SITES标准与国内标准规范的不匹配,分值权重的失衡,缺乏政府相关福利政策支持和推广受限制等问题。 展开更多
关键词 城市绿地 可持续景观 可持续场地倡议(siteS) 景观绩效
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Understanding Bridging Sites and Accelerating Quantum Efficiency for Photocatalytic CO_(2) Reduction 被引量:1
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作者 Kangwang Wang Zhuofeng Hu +8 位作者 Peifeng Yu Alina M.Balu Kuan Li Longfu Li Lingyong Zeng Chao Zhang Rafael Luque Kai Yan Huixia Luo 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第1期68-84,共17页
We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in... We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in S_(v)–In_(2)S_(3)@2H–MoTe_(2).The X-ray absorption near-edge structure shows that the formation of S_(v)–In_(2)S_(3)@2H–MoTe_(2) adjusts the coordination environment via interface engineering and forms Mo–S polarized sites at the interface.The interfacial dynamics and catalytic behavior are clearly revealed by ultrafast femtosecond transient absorption,time-resolved,and in situ diffuse reflectance–Infrared Fourier transform spectroscopy.A tunable electronic structure through steric interaction of Mo–S bridging bonds induces a 1.7-fold enhancement in S_(v)–In_(2)S_(3)@2H–MoTe_(2)(5)photogenerated carrier concentration relative to pristine S_(v)–In_(2)S_(3).Benefiting from lower carrier transport activation energy,an internal quantum efficiency of 94.01%at 380 nm was used for photocatalytic CO_(2)RR.This study proposes a new strategy to design photocatalyst through bridging sites to adjust the selectivity of photocatalytic CO_(2)RR. 展开更多
关键词 Quantum efficiency Electronic structure Steric interaction Bridging sites CO_(2)reduction
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Comparison of bone artifacts from the Schöningen site in Germany and the Lingjing site in China
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作者 WANG Hua LI Zhanyang Thijs van KOLFSCHOTEN 《人类学学报》 CSSCI CSCD 北大核心 2024年第2期214-232,共19页
Similarities play an important role in the reconstruction of human physical,cultural and technological evolution.The two sites presented in this paper,the Middle Palaeolithic site Lingjing in China Layer 10 and 11 and... Similarities play an important role in the reconstruction of human physical,cultural and technological evolution.The two sites presented in this paper,the Middle Palaeolithic site Lingjing in China Layer 10 and 11 and the Lower Palaeolithic site Schöningen 13Ⅱ-4,the socalled Schöningen Spear Horizon in Germany,show striking similarities.The archaeological record of both sites includes lithic artifacts as well as a very large assemblage of fossil bones.The preservation of the material at both sites is excellent and the faunas encountered at both sites show many similarities.The faunal lists of both sites include a diverse carnivore guild,an elephant species,two different rhinoceros species,two different equids,different cervids and large bovids.Both sites also yielded bone retouchers as well as a unique record of bone hammers that show identical,unusual flaking and percussion damage.These similarities are remarkable if one takes into account the difference in age(ca 200 kaBP)and the geographical distance between the two sites of ca 8000 km.Therefore,we do not assume a close cultural link between the hominin populations active at both sites.The authors assume that the observed similarities show more or less identical,opportunistic hominin behaviour at both sites located in a comparable environment with more or less similar taphonomic conditions. 展开更多
关键词 PALAEOLITHIC open-air sites bone tools Asia EUROPE
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Brønsted-acid sites induced photocatalytic cracking of low-polarity polyethylene plastics
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作者 Qianyou Wen Quan Zhang +6 位作者 Zhengzheng Liu Huining Wang Shuya Hao Fan Zhang Lijuan Zhang Qing Han Gengfeng Zheng 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第9期509-515,共7页
Polyolefins such as polyethylene(PE)are one of the largest-scale synthetic plastics and play a key role in modern society.However,polyethylene is extremely inert to chemical recycling owing to its lack of chemical fun... Polyolefins such as polyethylene(PE)are one of the largest-scale synthetic plastics and play a key role in modern society.However,polyethylene is extremely inert to chemical recycling owing to its lack of chemical functionality and low polarity,making it one of the most challenging environmental hazards globally.Herein,we developed a phosphorylated CeO_(2)catalyst by an organophosphate precursor and featured efficient photocatalysis of low-density polyethylene(LDPE)without the acid or alkaline pre-treatment.Compared to pristine CeO_(2),the surface phosphorylation allows to introduce Brønsted acid sites,which facilitate to form carbonium ions on LDPE via protonation.In addition,the suitable band structure of the phosphorylated CeO_(2)catalyst enables efficient photoabsorption and generates reactive oxygen species,leading to the C–C bond cleavage of LDPE.As a result,the phosphorylated CeO_(2)catalyst exhibited an outstanding carbon conversion rate of>94%after 48 h of photocatalysis under 50 mW/cm^(2)of simulated sunlight,with a high CO_(2)product selectivity of>99%.Furthermore,the PE microparticles with sizes larger than 10μm released from LDPE plastic wrap were directly and completely degraded by photocatalysis within 12 h,suggesting an attractive and environmentally benign strategy of utilizing solar energy-based photocatalysis for reducing potential hazards of LDPE plastic trashes. 展开更多
关键词 Photocatalytic cracking POLYETHYLENE Surface phosphorylation Bronsted-acid site Carbon conversion
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Effects of synthetic site water on bentonite-concrete system for a potential nuclear waste repository
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作者 Zhao Sun Yong-Gui Chen +3 位作者 Wei-Min Ye Qiong Wang Dong-Bei Wu Zhen-Yu Yin 《Journal of Rock Mechanics and Geotechnical Engineering》 SCIE CSCD 2024年第9期3786-3797,共12页
In high-level nuclear waste(HLW)repositories,concrete and compacted bentonite are designed to be employed as buffer materials,which may raise a problem of interactions between concrete and bentonite.These interactions... In high-level nuclear waste(HLW)repositories,concrete and compacted bentonite are designed to be employed as buffer materials,which may raise a problem of interactions between concrete and bentonite.These interactions would lead to mineralogy transformation and buffer performance decay of bentonite under the near field environment conditions in a repository.A small-scale experimental setup was established to simulate the concrete-bentonite-site water interaction system from a potential nuclear waste repository in China.Three types of mortars were prepared to correspond to the concrete at different degradation states.The results permit the determination of the following:(1)The macroproperties of Gaomiaozi(GMZ)bentonite(e.g.swelling pressure,permeability,the final dry density,and water content of reacted samples);(2)The composition evolution of fluids from the synthetic site water-concrete-bentonite interaction systems;(3)The sample characterization including Fourier transform infrared spectroscopy(FTIR)and X-ray powder diffraction(XRD).Under the infiltration of the synthesis Beishan site water(BSW),the swelling pressure of bentonite decreases slowly with time after reaching its second swelling peak.The flux decreases with time during the infiltrations,and it tends to be stable after more than 120 d.Due to the cation exchange reactions in the BSW-concrete-bentonite systems,the divalent cations(Ca and Mg)were consumed,and the monovalent cations(Na and K)were released.The dissolution of minerals in the bentonite such as albite causes Si increasing in the pore water.It was concluded that the hydro-mechanical property degradation of bentonite takes place when it comes into contact with concrete mortar,even under low-pH groundwater conditions.The soil dispersion,the uneven water content,and the uneven dry density in bentonite samples may partly contribute to the swelling decay of bentonite.Therefore,the direct contact with concrete has an obvious effect on the performance of bentonite. 展开更多
关键词 Mock-up device GMZ bentonite site water-concrete-bentonite system Geochemistry Buffer performance
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Effects of site preparation methods on soil physical properties and outplanting success of coniferous seedlings in boreal forests
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作者 Aleksey S.Ilintsev Elena N.Nakvasina Alexander P.Bogdanov 《Journal of Forestry Research》 SCIE EI CAS CSCD 2024年第2期70-80,共11页
This study assessed the effect of patch scarification and mounding on the physical properties of the root layer and the success of tree planting in various types of forests.This study was conducted on 12 forest sites ... This study assessed the effect of patch scarification and mounding on the physical properties of the root layer and the success of tree planting in various types of forests.This study was conducted on 12 forest sites in taiga forests of the European part of Russia.A total of 54 plots were set up to assess seedling survival;root collar diameter,height,and heigh increment were measured for 240 seedlings to assess growth.In the rooting layer,240 soil samples were taken to determine physical properties.The study showed that soil treatment methods had no effect on bulk density and total porosity in Cladina sites.However,reduced soil moisture was noted,particularly in mounds,resulting in increased aeration.In Myrtillus sites,there were increased bulk density,reduced soil moisture,and total porosity in the mounds.Mounding treatment in Polytrichum sites resulted in reduced soil moisture and increased aeration porosity.In the Myrtillus and Polytrichum sites,patch scarification had no effects on physical properties.In Polytrichum sites,survival rates,heights,and heigh increments of bareroot Norway spruce seedlings in mounds were higher than in patches;however,the same did not apply to diameter.In Cladina and Myrtillus sites,there was no difference in growth for bareroot and containerised seedlings with different soil treatments.Growing conditions and soil types should be considered when applying different soil treatment methods to ensure high survival rates and successful seedling growth. 展开更多
关键词 Boreal forests Mechanical site preparation Patch scarification MOUNDING Soil properties Containerised seedlings Bareroot seedlings
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PVDF-assisted pyrolysis strategy for corrugated plate oxygen electrocatalysis nanoreactor:Simultaneously realizing efficient active sites and rapid mass transfer
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作者 Chenxi Xu Liang Chen +6 位作者 Haihui Zhou Shifeng Qin Zhaohui Hou Yangyang Chen Jiale Sun Junwei Xu Zhongyuan Huang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第10期612-621,I0013,共11页
Though Zn-air batteries(ZABs)are one of the most promising system for energy storage and conversion,challenge still persists in its commercial application due to the sluggish kinetics of oxygen reduction/evolution rea... Though Zn-air batteries(ZABs)are one of the most promising system for energy storage and conversion,challenge still persists in its commercial application due to the sluggish kinetics of oxygen reduction/evolution reaction(ORR/OER).Hereby,a polyvinylidene fluoride(PVDF)-assisted pyrolysis strategy is proposed to develop a novel corrugated plate-like bifunctional electrocatalyst using two-dimensional zeolitic imidazolate frameworks(2D ZIF-67)as the precursor.The employed PVDF plays an important role in inheriting the original 2D structure of ZIF-67 and modulating the composition of the final products.As a result,a corrugated plate-like electrocatalyst,high-density Co nanoparticles decorated 2D Co,N,and F tri-doped carbon nanosheets,can be obtained.The acquired electrocatalyst enables efficient active sites and rapid mass transfer simultaneously,thus showing appreciable electrocatalytic performance for rechargeable Zn-air batteries.Undoubtedly,our proposed strategy offers a new perspective to the design of advanced oxygen electrocatalysts. 展开更多
关键词 Active sites Mass transfer Corrugated plate Oxygen electrocatalyst Zn-air batteries
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Efficient and reversible separation of NH_(3) by deep eutectic solvents with multiple active sites and low viscosities
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作者 Jiayin Zhang Lu Zheng +4 位作者 Siqi Fang Hongwei Zhang Zhenping Cai Kuan Huang Lilong Jiang 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第3期97-105,共9页
The efficient separation and collection of ammonia(NH_(3))during NH_(3) synthesis process is essential to improve the economic efficiency and protect the environment.In this work,ethanolammonium hydrochloride(EtOHACl)... The efficient separation and collection of ammonia(NH_(3))during NH_(3) synthesis process is essential to improve the economic efficiency and protect the environment.In this work,ethanolammonium hydrochloride(EtOHACl)and phenol(PhOH)were used to prepare a novel class of deep eutectic solvents(DESs)with multiple active sites and low viscosities.The NH_(3) separation performance of EtOHACl+PhOH DESs was analyzed completely.It is figured out that the NH_(3) absorption rates in EtOHACl+PhOH DESs are very fast.The NH_(3) absorption capacities are very high and reach up to 5.52 and 10.74 mol·kg1 at 11.2 and 100.4 kPa under 298.2 K,respectively.In addition,the EtOHACl+PhOH DESs present highly selective absorption of NH_(3) over N_(2) and H_(2) and good regenerative properties after seven cycles of absorption/desorption.The intrinsic separation mechanism of NH_(3) by EtOHACl+PhOH DESs was further revealed by spectroscopic analysis and quantum chemistry calculations. 展开更多
关键词 SEPARATION Absorption Ionic liquid Deep eutectic solvent Multiple active site Low viscosity
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Quantitative Analysis of Seeing with Height and Time at Muztagh-Ata Site Based on ERA5 Database
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作者 Xiao-Qi Wu Cun-Ying Xiao +3 位作者 Ali Esamdin Jing Xu Ze-Wei Wang Luo Xiao 《Research in Astronomy and Astrophysics》 SCIE CAS CSCD 2024年第1期87-95,共9页
Seeing is an important index to evaluate the quality of an astronomical site.To estimate seeing at the Muztagh-Ata site with height and time quantitatively,the European Centre for Medium-Range Weather Forecasts reanal... Seeing is an important index to evaluate the quality of an astronomical site.To estimate seeing at the Muztagh-Ata site with height and time quantitatively,the European Centre for Medium-Range Weather Forecasts reanalysis database(ERA5)is used.Seeing calculated from ERA5 is compared consistently with the Differential Image Motion Monitor seeing at the height of 12 m.Results show that seeing decays exponentially with height at the Muztagh-Ata site.Seeing decays the fastest in fall in 2021 and most slowly with height in summer.The seeing condition is better in fall than in summer.The median value of seeing at 12 m is 0.89 arcsec,the maximum value is1.21 arcsec in August and the minimum is 0.66 arcsec in October.The median value of seeing at 12 m is 0.72arcsec in the nighttime and 1.08 arcsec in the daytime.Seeing is a combination of annual and about biannual variations with the same phase as temperature and wind speed indicating that seeing variation with time is influenced by temperature and wind speed.The Richardson number Ri is used to analyze the atmospheric stability and the variations of seeing are consistent with Ri between layers.These quantitative results can provide an important reference for a telescopic observation strategy. 展开更多
关键词 site testing atmospheric effects methods:data analysis telescopes EARTH
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The suitability assessment on site selection for bottom seeding scallop culture based on analytic hierarchy process
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作者 Ziniu ZHANG Zhenyan WANG +2 位作者 Guihua LI Meihan ZHAO Wenjian LI 《Journal of Oceanology and Limnology》 SCIE CAS CSCD 2024年第2期647-663,共17页
Scallop culture is an important way of bottom-seeding marine ranching,which is of great significance to improve the current situation of fishery resources.However,there are some problems in site-selection evaluation o... Scallop culture is an important way of bottom-seeding marine ranching,which is of great significance to improve the current situation of fishery resources.However,there are some problems in site-selection evaluation of marine ranching,such as imperfect criteria system,complex structure,untargeted criteria quantification,etc.In addition,no site-selection evaluation method of bottom-seeding culture areas for scallops is available.Therefore,we established a hierarchy structure model according to the analytic hierarchy process(AHP)theory,in which social,physical,chemical,and biological environments are used as main criteria,and marine functional zonation,water depth,current,water temperature,salinity,substrate type,water quality,sediment quality,red tide,phytoplankton,and zooplankton are used as sub-criteria,on which a multi-parameter evaluation system is set up.Meanwhile,the dualism method,assignment method,and membership function method were used to quantify sub-criteria,and a quantitative evaluation for the entire criteria was added,including the evaluation and analysis of two types of unsuitable environmental situations.By overall consideration in scallop yield,quality,and marine ranching construction objectives,the weight of the main criteria could be determined.Five grades in the suitability corresponding to the evaluation result were divided,and the Python language was used to create an evaluation system for efficient calculation and intuitive presentation of the evaluation outcome.Eight marine cases were simulated based on existing survey data,and the results prove that the method is feasible for evaluating and analyzing the site selection of bottom-seeding culture areas for scallops under various environmental situations.The proposed evaluation method can be promoted for the site selection of bottom-seeding marine ranching.This study provided theoretical and methodological references for the site selection evaluation of other types of marine ranching. 展开更多
关键词 marine ranching bottom-seeding scallops site selection evaluation analytic hierarchy process evaluation system
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Ni/ZSM-5 Catalysts for Light Olefin Oligomerization:Effects of Supports and Ni Sites on Activity and Selectivity
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作者 Zuo Qi Liang Ke +5 位作者 Ma Yirong Jia Yangxiao Liao Mingjie Zheng Jiajun Li Ruifeng Li Wenlin 《China Petroleum Processing & Petrochemical Technology》 SCIE CAS CSCD 2024年第3期15-23,共9页
A series of Ni/ZSM-5 containing a small amount of Ni was prepared by an ion exchanged method.The impact of the n(SiO_(2))/n(Al_(2)O_(3))ratio on the catalytic activity was studied using the samples 0.09Ni/ZSM-5(60)and... A series of Ni/ZSM-5 containing a small amount of Ni was prepared by an ion exchanged method.The impact of the n(SiO_(2))/n(Al_(2)O_(3))ratio on the catalytic activity was studied using the samples 0.09Ni/ZSM-5(60)and 0.09Ni/ZSM-5(130).To determine the interaction between the Ni species and acid sites on the surface of the catalyst,the catalysts were characterized by N2 adsorption-desorption,X-ray diffraction(XRD),scanning electron microscopy(SEM),and UV-vis spectroscopy.The performance of the catalysts for the catalytic oligomerization of 1-hexene was investigated in detail.The nickel species were found to be uniformly distributed in all the catalysts.It was discovered that the oligomerization activity of the catalyst can be improved using Ni species;however,the contribution of Brønsted acids in oligomerization reactions is greater than that of Ni sites and Lewis acids. 展开更多
关键词 nickel ZEOLITE acid sites OLIGOMERIZATION catalyst
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Boost the Utilization of Dense FeN_(4) Sites for High-Performance Proton Exchange Membrane Fuel Cells
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作者 Yanrong Li Shuhu Yin +4 位作者 Long Chen Xiaoyang Cheng Chongtai Wang Yanxia Jiang Shigang Sun 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2024年第3期398-405,共8页
Iron-nitrogen-carbon(Fe-N-C)catalysts for the oxygen reduction reaction(ORR)in proton exchange membrane fuel cells(PEMFCs)have seriously been hindered by their poor ORR performance of Fe-N-C due to the low active site... Iron-nitrogen-carbon(Fe-N-C)catalysts for the oxygen reduction reaction(ORR)in proton exchange membrane fuel cells(PEMFCs)have seriously been hindered by their poor ORR performance of Fe-N-C due to the low active site density(SD)and site utilization.Herein,we reported a melamine-assisted vapor deposition approach to overcome these hindrances.The melamine not only compensates for the loss of nitrogen caused by high-temperature pyrolysis but also effectively etches the carbon substrate,increasing the external surface area and mesoporous porosity of the carbon substrate.These can provide more useful area for subsequent vapor deposition on active sites.The prepared 0.20Mela-FeNC catalyst shows a fourfold higher SD value and site utilization than the FeNC without the treatment of melamine.As a result,0.20Mela-FeNC catalyst exhibits a high ORR activity with a half-wave potential(E_(1/2))of 0.861 V and 12-fold higher ORR mass activity than the FeNC in acidic media.As the cathode in a H_(2)-O_(2)PEMFCs,0.20Mela-FeNC catalyst demonstrates a high peak power density of 1.30 W cm^(-2),outstripping most of the reported Fe-N-C catalysts.The developed melamine-assisted vapor deposition approach for boosting the SD and utilization of Fe-N-C catalysts offers a new insight into high-performance ORR electrocatalysts. 展开更多
关键词 fuel cells MELAMINE oxygen reduction reaction site density UTILIZATION
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Structural engineering of Fe single-atom oxygen reduction catalyst with high site density and improved mass transfer
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作者 Jiawen Wu Yuanzhi Zhu +3 位作者 An Cai Xiaobin Fan Wenchao Peng Yang Li 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第11期634-644,共11页
Fe-N-C catalysts are widely considered as promising non-precious-metal candidates for electrocatalytic oxygen reduction reaction(ORR),Yet despite their high catalytic activity through rational modulation,challenges re... Fe-N-C catalysts are widely considered as promising non-precious-metal candidates for electrocatalytic oxygen reduction reaction(ORR),Yet despite their high catalytic activity through rational modulation,challenges remain in their low site density and unsatisfactory mass transfer structure.Herein,we present a structural engineering approach employing a soft-template coating strategy to fabricate a hollow and hierarchically porous N-doped carbon framework anchored with atomically dispersed Fe sites(FeNCh) as an efficient ORR catalyst.The combination of hierarchical porosity and high exterior surface area is proven crucial for exposing more active sites,which gives rise to a remarkable ORR performance with a half-wave potential of 0.902 V in 0.1 m KOH and 0.814 V in 0.1 m HClO_(4),significantly outperforming its counterpart with solid structure and dominance of micropores(FeNC-s).The mass transfer property is revealed by in-situ electrochemical impedance spectroscopy(EIS) measurement.The distribution of relaxation time(DRT) analysis is further introduced to deconvolve the kinetic and mass transport processes,which demonstrates an alleviated mass transport resistance for FeNC-h,validating the effectiveness of structural engineering.This work not only provides an effective structural engineering approach but also contributes to the comprehensive mass transfer evaluation on advanced electrocatalyst for energy conversion applications. 展开更多
关键词 Single-atom catalysts Oxygen reduction reaction Structural engineering Active site density Mass transfer Zinc-air batteries
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Regulating metal-acid double site balance on mesoporous SiO_(2)-Al_(2)O_(3) composite oxide for supercritical n-decane cracking
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作者 Liu-Ling Chen Jun Zhang +5 位作者 Chun-Guang Li Li-Qun Fei Bo Wang Chen-Qi Zhang Yi Jiao Jian-Li Wang 《Petroleum Science》 SCIE EI CAS CSCD 2024年第4期2881-2891,共11页
The balance between metal and acid sites directly affects the preparation of high-performance cracking catalysts with high heat sink and low coking.Nevertheless,how to control acid-metal sites balance and its relation... The balance between metal and acid sites directly affects the preparation of high-performance cracking catalysts with high heat sink and low coking.Nevertheless,how to control acid-metal sites balance and its relationship with cracking performance are reported scarcely.In this work,a series of Pt/Al_(2)O_(3)-SiO_(2) dual sites catalysts with different metal to acid active sites ratio(C_(M)/C_(SA))were constructed by ethanolassisted impregnation method and the impact on n-decane cracking under supercritical conditions was systematically and deeply investigated.The results showed that the conversion and carbon deposition increased gradually with varied C_(M)/C_(SA)and reached the balance at C_(M)/C_(SA)of 0.13.The proper ratio C_(M)/C_(SA)(0.13)can balance the deep dehydrogenation coking over metal active sites and high heat sink of cracking over acid active sites,the chemical heat sink reaches amazing 1.75 MJ/kg and carbon deposition is only22.03 mg/cm^(2) at 750℃.Meanwhile,the few metal sites at low C_(M)/C_(SA)and the few strong acid sites at high C_(M)/C_(SA)are the main factors limiting the cracking activity.Low C_(M)/C_(SA)limit the activation of C-H bond and deep dehydrogenation of coking precursor,resulting in relative low cracking activity and carbon deposition,while high C_(M)/C_(SA)limit the activation of C-C bond and increase the deep dehydrogenation.In this contribution,design and construction of metal-acid dual sites can not only provide the technical solution for the preparation of high heat sink and low coking cracking catalyst,but also deepen the understanding of the cracking path of hydrocarbon fuel. 展开更多
关键词 Metal-acid dual sites balance Catalytic cracking Hydrocarbon fuels Chemical heat sink Carbon deposition
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Building Fe atom–cluster composite sites using a site occupation strategy to boost electrochemical oxygen reduction
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作者 Tingyi Zhou Yi Guan +9 位作者 Changjie He Lei Zhang Xueliang Sun Zhongxin Song Qianling Zhang Chuanxin He Xiantao Jiang Zhaoyan Luo Wei Xing Xiangzhong Ren 《Carbon Energy》 SCIE EI CAS CSCD 2024年第3期276-286,共11页
The high-temperature pyrolysis process for preparing M–N–C single-atom catalyst usually results in high heterogeneity in product structure concurrently contains multiscale metal phases from single atoms(SAs),atomic ... The high-temperature pyrolysis process for preparing M–N–C single-atom catalyst usually results in high heterogeneity in product structure concurrently contains multiscale metal phases from single atoms(SAs),atomic clusters to nanoparticles.Therefore,understanding the interactions among these components,especially the synergistic effects between single atomic sites and cluster sites,is crucial for improving the oxygen reduction reaction(ORR)activity of M–N–C catalysts.Accordingly,herein,we constructed a model catalyst composed of both atomically dispersed FeN4 SA sites and adjacent Fe clusters through a site occupation strategy.We found that the Fe clusters can optimize the adsorption strength of oxygen reduction intermediates on FeN4 SA sites by introducing electron-withdrawing–OH ligands and decreasing the d-band center of the Fe center.The as-developed catalyst exhibits encouraging ORR activity with halfwave potentials(E1/2)of 0.831 and 0.905 V in acidic and alkaline media,respectively.Moreover,the catalyst also represents excellent durability exceeding that of Fe–N–C SA catalyst.The practical application of Fe(Cd)–CNx catalyst is further validated by its superior activity and stability in a metalair battery device.Our work exhibits the great potential of synergistic effects between multiphase metal species for improvements of singleatom site catalysts. 展开更多
关键词 d-band center metal clusters oxygen reduction reaction single-atom catalyst site occupations strategy
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Surgical site infection following pancreaticoduodenectomy in a referral cancer center in Mexico
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作者 Rodrigo Villaseñor-Echavarri Javier Melchor-Ruan +5 位作者 Mercedes Aranda-Audelo Gabriela Arredondo-Saldaña Patricia Volkow-Fernandez Maria del Carmen Manzano-Robleda Alejandro E Padilla-Rosciano Diana Vilar-Compte 《Hepatobiliary & Pancreatic Diseases International》 SCIE CAS CSCD 2024年第5期502-508,共7页
Background: Pancreaticoduodenectomy is the standard treatment for resectable periampullary cancer. Surgical site infections(SSI) are common complications with increased morbidity. The study aimed to describe the preva... Background: Pancreaticoduodenectomy is the standard treatment for resectable periampullary cancer. Surgical site infections(SSI) are common complications with increased morbidity. The study aimed to describe the prevalence, risk factors, microbiology, and outcomes of SSI among patients undergoing pancreaticoduodenectomy. Methods: We conducted a retrospective study in a referral cancer center between January 2015 and June 2021. We analyzed baseline patient characteristics and SSI occurrence. Culture results and susceptibility patterns were described. Multivariate logistic regression was used to determine risk factors, proportional hazards model to evaluate mortality, and Kaplan-Meier analysis to assess long-term survival. Results: A total of 219 patients were enrolled in the study;101(46%) developed SSI. Independent factors for SSI were diabetes mellitus, preoperative albumin level, biliary drainage, biliary prostheses, and clinically relevant postoperative pancreatic fistula. The main pathogens were Enterobacteria and Enterococci. Multidrug-resistance rate in SSI was high but not associated with increased mortality. Infected patients had higher odds of sepsis, longer hospital stay and intensive care unit stay, and readmission rate. Neither 30-day mortality nor long-term survival was significantly different between infected and non-infected patients. Conclusions: SSI prevalence among patients undergoing pancreaticoduodenectomy was high and largely caused by resistant microorganisms. Most risk factors were related to preoperative instrumentation of the biliary tree. SSI was associated with greater risk of unfavorable outcomes;however, survival was unaffected. 展开更多
关键词 Surgical site infection PANCREATICODUODENECTOMY Pancreatic cancer Endoscopic biliary drainage Biliary prosthesis
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Rapid detection and risk assessment of soil contamination at lead smelting site based on machine learning
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作者 Sheng-guo XUE Jing-pei FENG +5 位作者 Wen-shun KE Mu LI Kun-yan QIU Chu-xuan LI Chuan WU Lin GUO 《Transactions of Nonferrous Metals Society of China》 SCIE EI CAS CSCD 2024年第9期3054-3068,共15页
A general prediction model for seven heavy metals was established using the heavy metal contents of 207soil samples measured by a portable X-ray fluorescence spectrometer(XRF)and six environmental factors as model cor... A general prediction model for seven heavy metals was established using the heavy metal contents of 207soil samples measured by a portable X-ray fluorescence spectrometer(XRF)and six environmental factors as model correction coefficients.The eXtreme Gradient Boosting(XGBoost)model was used to fit the relationship between the content of heavy metals and environment characteristics to evaluate the soil ecological risk of the smelting site.The results demonstrated that the generalized prediction model developed for Pb,Cd,and As was highly accurate with fitted coefficients(R^(2))values of 0.911,0.950,and 0.835,respectively.Topsoil presented the highest ecological risk,and there existed high potential ecological risk at some positions with different depths due to high mobility of Cd.Generally,the application of machine learning significantly increased the accuracy of pXRF measurements,and identified key environmental factors.The adapted potential ecological risk assessment emphasized the need to focus on Pb,Cd,and As in future site remediation efforts. 展开更多
关键词 smelting site potentially toxic elements X-ray fluorescence potential ecological risk machine learning
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Electrocatalysts with atomic-level site for nitrate reduction to ammonia
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作者 Shuai Yin Rong Cao +4 位作者 Yifan Han Jiachangli Shang Jing Zhang Wei Jiang Guigao Liu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第9期642-668,共27页
Ammonia(NH_(3))is an important raw material for modern agriculture and industry,being widely demanded to sustain the sustainable development of modern society.Currently,the industrial production methods of NH_(3),such... Ammonia(NH_(3))is an important raw material for modern agriculture and industry,being widely demanded to sustain the sustainable development of modern society.Currently,the industrial production methods of NH_(3),such as the traditional Haber-Bosch process,have drawbacks including high energy consumption and significant carbon dioxide emissions.In recent years,the electrocatalytic nitrate reduction reaction(NO_(3)RR)powered by intermittent renewable energy sources has gradually become a multidisciplinary research hotspot,as it allows for the efficient synthesis of NH_(3)under mild conditions.In this review,we focus on the research of electrocatalysts with atomic-level site,which have attracted attention due to their extremely high atomic utilization efficiency and unique structural characteristics in the field of NO_(3)RR.Firstly,we introduce the mechanism of nitrate reduction for ammonia synthesis and discuss the in-situ characterization techniques related to the mechanism study.Secondly,we review the progress of the electrocatalysts with atomic-level site for nitrate reduction and explore the structure-activity relationship to guide the rational design of efficient catalysts.Lastly,the conclusions of this review and the challenges and prospective of this promising field are presented. 展开更多
关键词 Ammonia synthesis Nitrate reduction Electrocatalysts with atomic-level site Reaction mechanism In-situ characterization techniques
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