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Correcting Errors in the Adsorbed Intermediates of CO_(2)Electroreduction
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作者 Ricardo Urrego-Ortiz Camberly Schaffer Zhong +3 位作者 Wei Jie Teh Santiago Builes Boon Siang Yeo Federico Calle-Vallejo 《Carbon Energy》 2026年第2期271-283,共13页
Density functional theory(DFT)has helped propel the advance of electrocatalysis in the past two decades.In view of its massive use,it is worth asking how reliable DFT is for the prediction of adsorption energies,which... Density functional theory(DFT)has helped propel the advance of electrocatalysis in the past two decades.In view of its massive use,it is worth asking how reliable DFT is for the prediction of adsorption energies,which are paramount in computational electrocatalysis models.Here,we provide an experimental-computational approach to break down overall adsorption-energy errors into separate gas-phase and adsorbed-phase contributions.The method is evaluated using experimental data and various exchange-correlation functionals and materials for C-and O-containing species.Our main conclusion is that no functional is simultaneously accurate for adsorbates and molecules,as adsorbed-phase errors are visibly different from gas-phase errors.Importantly,total,gas-phase,and adsorbed-phase errors are correlated,revealing intrinsic DFT limitations and enabling the elaboration of swift correction routines.To illustrate the benefits of our approach,we deconvolute and correct all errors in CO_(2)electroreduction to CO and find an agreement with experiments close to chemical accuracy for numerous transition-metal electrodes and all scrutinized functionals. 展开更多
关键词 adsorption energieswhich adsorption energies density functional theory dft computational electrocatalysis density functional theory adsorbed intermediates computational electrocatalysis modelsherewe experimental data
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Process analysis of nuclear hydrogen production via intermediate temperature SOEC electrolysis
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作者 Qing Shao Yue Lu +7 位作者 Dun Jin Ling-Hong Luo Xiu-Lin Wang Hui-Chao Yao Ruo-Yun Dai Cheng-Zhi Guan Guo-Ping Xiao Jian-Qiang Wang 《Nuclear Science and Techniques》 2026年第2期122-133,共12页
When the operating temperature of a solid oxide electrolysis cell(SOEC)is lower than the outlet temperature of a nuclear reactor,the reactor can be directly coupled with the SOEC as a high-temperature heat source.Howe... When the operating temperature of a solid oxide electrolysis cell(SOEC)is lower than the outlet temperature of a nuclear reactor,the reactor can be directly coupled with the SOEC as a high-temperature heat source.However,the key to the efficiency and return on investment of this hybrid energy system lies in the expected lifetime of the SOEC.This study assessed Ni-YSZ|YSZ|GDC|LSC fuel electrode support cells’long-term stability during electrolysis at 650℃with a current density of−0.5Acm^(−2)over 1818 h.The average voltage degradation rate of 2.63%kh^(−1)unfolded in two phases:an initial rapid decay(90 to 1120 h at 3.58%kh^(−1))and a stable decay(1120 to 1818 h at 2.14%kh^(−1)),emphasizing SOECs’probability coupling with nuclear reactors at 650℃.Post-1818-hour electrolysis revealed nickel particle formation associated with Ni(OH)_(x)diffusion and re-deposition,alongside a strontium-containing layer causing interface cracking.Despite minimal strontium segregation in the EDS,XPS data indicated surface segregation of Sr.This study provides crucial insights into prolonged SOEC operation,highlighting both its potential and challenges. 展开更多
关键词 Nuclear hydrogen production SOEC STABILITY intermediate temperature
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Effects of intermediate principal stress on strainburst in granite:Insights from true-triaxial unloading experiments and PFC3D-GBM simulations
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作者 Hongru Li Manchao He +4 位作者 Tai Cheng Yafei Qiao Dongqiao Liu Jie Hu Yingming Xiao 《International Journal of Mining Science and Technology》 2026年第2期295-311,共17页
To improve the accuracy of rockburst risk evaluation in mining and tunnelling engineering,the influence of intermediate principal stress σ_(2) deserves further consideration,which has been neglected in general predic... To improve the accuracy of rockburst risk evaluation in mining and tunnelling engineering,the influence of intermediate principal stress σ_(2) deserves further consideration,which has been neglected in general prediction frameworks.This study employs an integrated approach that combines true-triaxial unloading experiments with three-dimensional grain-based discrete element modeling(PFC3D-GBM)to examine the effects of σ_(2) on strain systematically burst and elucidate the underlying mechanisms.Through this dual experimental–numerical methodology,the strainburst characteristics under varying σ_(2) are analyzed in detail regarding mechanical responses,failure evolution and patterns,microscope fracture mechanisms,and energy partitioning.The results indicate that elevated σ_(2) can enhance the bearing capacity of rock,thereby necessitating a higher stress condition required for strainburst.However,it also enlarges the potential strainburst intensity,manifesting as deeper rockburst pits and more violent ejection of rock fragments.An increasing σ_(2) facilitates the microscope transgranular fractures,inhibits intergranular tensile fractures,and raises the kinetic energy conversion ratio slightly.It affects the intensity of strainburst through the following mechanisms,including the increase of energy storage limit,the intensification of Poisson effect for lateral expansion,and the enhancement of the transgranular fracturing mechanism.In practical engineering,the depth and range of support needs to be ensured under high σ_(2) conditions,and it is recommended to use prestressing techniques to control the development of significant slabbing. 展开更多
关键词 ROCKBURST intermediate principal stress True-triaxial experiment 3D grain-based model
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Barrierless reactions of C2 Criegee intermediates with H_(2)SO_(4)and their implication to oligomers and new particle formation 被引量:1
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作者 Yang Cheng Chao Ding +6 位作者 Tianlei Zhang Rui Wang Ruxue Mu Zeyao Li Rongrong Li Juan Shi Chongqin Zhu 《Journal of Environmental Sciences》 2025年第3期574-584,共11页
The formation of oligomeric hydrogen peroxide triggered by Criegee intermediate maybe contributes significantly to the formation and growth of secondary organic aerosol(SOA).However,to date,the reactivity of C2 Criege... The formation of oligomeric hydrogen peroxide triggered by Criegee intermediate maybe contributes significantly to the formation and growth of secondary organic aerosol(SOA).However,to date,the reactivity of C2 Criegee intermediates(CH_(3)CHOO)in areas contaminated with acidic gas remains poorly understood.Herein,high-level quantum chemical calculations and Born-Oppenheimer molecular dynamics(BOMD)simulations are used to explore the reaction of CH_(3)CHOO and H_(2)SO_(4)both in the gas phase and at the airwater interface.In the gas phase,the addition reaction of CH_(3)CHOO with H_(2)SO_(4)to generate CH_(3)HC(OOH)OSO_(3)H(HPES)is near-barrierless,regardless of the presence of water molecules.BOMD simulations showthat the reaction at the air-water interface is even faster than that in the gas phase.Further calculations reveal that the HPES has a tendency to aggregate with sulfuric acids,ammonias,and water molecules to form stable clusters,meanwhile the oligomerization reaction of CH_(3)CHOO with HPES in the gas phase is both thermochemically and kinetically favored.Also,it is noted that the interfacial HPES−ion can attract H_(2)SO_(4),NH_(3),(COOH)_(2)and HNO_(3)for particle formation from the gas phase to the water surface.Thus,the results of this work not only elucidate the high atmospheric reactivity of C2 Criegee intermediates in polluted regions,but also deepen our understanding of the formation process of atmospheric SOA induced by Criegee intermediates. 展开更多
关键词 Criegee intermediates H_(2)SO_(4) Atmospheric behavior Air-water interface Chemical processes
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Electron Paramagnetic Resonance(EPR)Studies of Photocatalytic Halogen Atom Transfer Intermediates Involving Organic Amines and Its Applications
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作者 Jin Weijun Ren Ke +1 位作者 Zhang Guanglu Jiang Min 《有机化学》 北大核心 2025年第10期3866-3872,共7页
In situ electron paramagnetic resonance(EPR)monitoring of the photocatalytic halogen atom transfer(XAT)reaction with organic amines has provided insights into the dynamic transformations of intermediates,including cat... In situ electron paramagnetic resonance(EPR)monitoring of the photocatalytic halogen atom transfer(XAT)reaction with organic amines has provided insights into the dynamic transformations of intermediates,including catalyst intermediate states,amine alkyl radicals,and the dehalogenation of halogenated hydrocarbons to form carbon-centered radicals.This approach facilitated the photocatalytic single-linear state oxygen-promoted halogen atom transfer quinoxalinone alkylation reaction. 展开更多
关键词 electron paramagnetic resonance(EPR) reaction intermediates halogen atom transfer(XAT) PHOTOCATALYST ALKYLATION
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Photocontrolled Solution[2+2]Polymerization of p-Phenylenediacrylate and Depolymerization
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作者 Miao-Yan Yi Yu Jiang Sai-Hu Liao 《Chinese Journal of Polymer Science》 2025年第11期1973-1980,I0007,共9页
The[2+2]photopolymerization of bisolefinic monomers is an important method for the synthesis of polymeric materials.However,these processes are usually carried out in solid states under the irradiation of high-energy ... The[2+2]photopolymerization of bisolefinic monomers is an important method for the synthesis of polymeric materials.However,these processes are usually carried out in solid states under the irradiation of high-energy UV light,while the corresponding[2+2]polymerization in solution has proved to be inefficient due to the lack of preassembly of the monomers.Herein,we demonstrate that the[2+2]polymerization of p-phenylenediacrylate monomers can be achieved in solution under visible light by employing energy transfer catalysis with 2,2'-methoxythioxanthone as a photocatalyst.Because no preassembly is required,this solution polymerization is applicable to p-phenylenediacrylate monomers with different ester groups,affording a series of cyclobutane-imbedded full-carbon chain polymers with high thermal stability,good solubility,and processibility.In addition,by virtue of the reversibility of the photo[2+2]cycloaddition,this[2+2]photopolymerization product can also undergo depolymerization to lower molecular weight polymers,suggesting the potential of this class of photopolymerization in the development of closed-loop chemical recyclable polymers. 展开更多
关键词 [2+2]Polymerization PHOTOPOLYMERIZATION p-Phenylenediacrylates ORGANOCATALYSIS depolymerization
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β-sheet Engineering of IsPETase for PET Depolymerization
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作者 Songfeng Gao Lixia Shi +8 位作者 Hongli Wei Pi Liu Wei Zhao Lanyu Gong Zijian Tan Huanhuan Zhai Weidong Liu Haifeng Liu Leilei Zhu 《Engineering》 2025年第4期180-193,共14页
The enzymatic depolymerization of polyethylene terephthalate(PET)offers a sustainable approach for the recycling of PET waste.Great efforts have been devoted to engineering PET depolymerases on the substrate binding c... The enzymatic depolymerization of polyethylene terephthalate(PET)offers a sustainable approach for the recycling of PET waste.Great efforts have been devoted to engineering PET depolymerases on the substrate binding cleft and the surrounding loops/α-helices on the surface.Here,we report the systematic engineering of whole β-sheet regions in the core of IsPETase(a PETase from Ideonella sakaiensis)via a fluorescent high-throughput screening assay.Twenty-one beneficial substitutions were obtained and iteratively recombined.The best variant,DepoPETase β,with an increase in the melting temperatures(T_(m))of 22.9℃,exhibited superior depolymerization performance and enabled complete depolymerization of100.5 g of untreated post-consumer PET(pc-PET;0.26% W_(enzyme)/W_(PET) enzyme loading)in liter-scale bioreactor at 50℃within 4 d.Crystallization and molecular dynamics simulations revealed that the improved activity and thermostability of DepoPETase β were due to enhanced hydrogen bonds and salt bridges in the β-sheet region,a more tightly packed structure of the core sheets and the surrounding helix,and improved binding of PET to the active sites.This study not only demonstrates the importance of engineering strategy in theβ-sheet region of PET hydrolases but also provides a potential PET depolymerase for large-scale PET recycling. 展开更多
关键词 Directed evolution High-throughput screening PETase PET depolymerization Thermostability β-sheet engineering
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Depolymerization and Functionalization of Super Engineering Plastics
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作者 Boning Gu Rui Huang +1 位作者 Yinsong Zhao Xuefeng Jiang 《Chinese Journal of Polymer Science》 2025年第6期876-886,I0006,共12页
Chemical recycling/upcycling of plastics has emerged as one of the most promising strategies for the plastic circular economy,enabling the depolymerization and functionalization of plastics into valuable monomers and ... Chemical recycling/upcycling of plastics has emerged as one of the most promising strategies for the plastic circular economy,enabling the depolymerization and functionalization of plastics into valuable monomers and chemicals.However,studies on the depolymerization and functionalization of challenging super engineering plastics have remained in early stage and underexplored.In this review,we would like to discuss the representative accomplishments and mechanism insights on chemical protocols achieved in depolymerization of super engineering plastics,especially for poly(phenylene sulfide)(PPS),poly(aryl ether)s including poly(ether ether ketone)(PEEK),polysulfone(PSU),polyphenylsulfone(PPSU)and polyethersulfone(PES).We anticipate that this review will provide an overall perspective on the current status and future trends of this emerging field. 展开更多
关键词 Super engineering plastics Chemical recycling/upcycling depolymerization FUNCTIONALIZATION
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Depolymerization of lignin over heterogeneous Co-NC catalyst
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作者 Fei Song Kai Du +6 位作者 Huamei Yang Qi Luo Yuxuan Liu Qian Qiang Yangming Ding Qingda An Changzhi Li 《Journal of Environmental Sciences》 2025年第6期654-663,共10页
Green and atom-economic depolymerization of lignin remains a great challenge due toits complex non-repetitive structure and the inert property for chemo-digestion. A redoxneutrallignin depolymerization system without ... Green and atom-economic depolymerization of lignin remains a great challenge due toits complex non-repetitive structure and the inert property for chemo-digestion. A redoxneutrallignin depolymerization system without the use of extra oxidant and/or reductantover a Co-NC catalyst has been developed in this work, providing the first non-noble metalheterogeneous catalytic system for redox-neutral valorization of lignin. Mechanistic studiesbased on control reactions and deuterium labeling experiments suggest that the reactionproceeds via ametal-catalyzed dehydrogenation of C_(α)-OH to afford a carbonyl intermediate,followed by C_(β)-O bond cleavage (via hydrogenolysis) to afford monophenols and aromaticketone products. The hydrogen used for the cleavage of the C_(β)-O bond originates from thealcoholmoiety in the substrate, and the cascade dehydrogenation and hydrogenolysis stepsare highly coupled, rendering it an efficient and atom-economic process. 展开更多
关键词 LIGNIN β-O-4 model compounds depolymerization Co-NC Mild conditions Aromatic chemical
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Adaptive phosphorus modulation tailoring hydroxyl intermediate adsorption for ultrafast water splitting
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作者 Jialin Zhang Liang Zhang +5 位作者 Chao Meng Lei Zhao Deyu Kong Jianglong Ji Xuemin Chen Yue Zhou 《Journal of Energy Chemistry》 2025年第10期438-447,共10页
Addressing inadequate OH^(*)adsorption in Ru Co alloy catalysts is crucial for boosting intermediate coverage and redirecting the water-splitting pathway.Herein,the adaptive P sites were strategically incorporated to ... Addressing inadequate OH^(*)adsorption in Ru Co alloy catalysts is crucial for boosting intermediate coverage and redirecting the water-splitting pathway.Herein,the adaptive P sites were strategically incorporated to overcome the aforementioned challenge.The P sites,as potent OH^(*)adsorption centers,synergize with Co sites to promote water dissociation and enrich surrounding Ru sites with H*intermediates,thus triggering the Volmer-Tafel route for hydrogen evolution reaction(HER).Besides,during the oxygen evolution reaction(OER),the surface of P-Ru Co was reconstructed into Ru-doped Co OOH with anchored PO_(4)^(3-).These PO_(4)^(3-)not only circumvent the intrinsic OH^(*)adsorption limitations of Ru-Co OOH in the adsorbate evolution mechanism(AEM)by rerouting to a more expeditious lattice oxygen oxidation mechanism(LOM)but also improve the coverage of key oxygen-containing intermediates,significantly accelerating OER kinetics.Consequently,the P-Ru Co demonstrates exceptional bifunctional performance,with overpotentials of 29 m V for HER and 222 m V for OER at 10 m A cm^(-2).Remarkably,the mass activities of PRu Co for HER(5.48 A mg^(-1))and OER(2.13 A mg^(-1))are 6.2 and 11.2 times higher than those of its commercial counterparts(Ru/C for HER and RuO_(2)for OER),respectively.When integrated into an anionexchange-membrane electrolyzer,this catalyst achieves ampere-level current densities of 1.32 A cm^(-2)for water electrolysis and 1.23 A cm^(-2)for seawater electrolysis at 2.1 V,with a 500-h durability. 展开更多
关键词 Water splitting Ampere-level current density Adaptive phosphorus modulation Hydroxyl intermediate adsorption RuCo alloy
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The intermediate water in the Philippine Sea 被引量:2
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作者 ZANG Nan WANG Fan SPRINTALL Janet 《Journal of Oceanology and Limnology》 SCIE CAS CSCD 2020年第5期1343-1353,共11页
The dimensional and temporal distribution of Antarctic Intermediate Water(AAIW)and North Pacifi c Intermediate Water(NPIW)in the Philippine Sea were explored using Argo profi les and gridded Argo data.As the salinity ... The dimensional and temporal distribution of Antarctic Intermediate Water(AAIW)and North Pacifi c Intermediate Water(NPIW)in the Philippine Sea were explored using Argo profi les and gridded Argo data.As the salinity minimum of intermediate water from mid-high latitude of the southern and northern hemisphere of the Pacifi c Ocean,the properties of AAIW and NPIW merge at about 10°N with diff erent properties in the Philippine Sea.The core of AAIW is located below 600 dbar with potential density of 27≤σθ≤27.3 kg/m 3 and salinity of 34.5≤S≤34.55.The core of NPIW is located between 300–700 dbar with potential density of 26.2≤σθ≤27 kg/m 3 and salinity of 34≤S≤34.4.The volume of AAIW and NPIW during January 2004 to December 2017 is negatively correlated.The time series of AAIW and NPIW is dominated by signifi cant periods of 6 and 8 months,respectively.The variations of AAIW and NPIW are mainly aff ected by volume transport through a 130°E section by the North Equatorial Current(NEC)and North Equatorial Undercurrent(NEUC). 展开更多
关键词 the intermediate water the Antarctic intermediate Water the North Pacifi c intermediate Water seasonal variation
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Influence of orientation of the intermediate principal stress on fracture reactivation in granite 被引量:1
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作者 Wei Wang Fanzhen Meng +6 位作者 Zhufeng Yue Guanghao Cui Qijin Cai Zhiyuan Li Dongliang Tian Hui Zhou Zaiquan Wang 《Journal of Rock Mechanics and Geotechnical Engineering》 2025年第2期859-876,共18页
Fracture(fault)reactivation can lead to dynamic geological hazards including earthquakes,rock collapses,landslides,and rock bursts.True triaxial compression tests were conducted to analyze the fracture reactivation pr... Fracture(fault)reactivation can lead to dynamic geological hazards including earthquakes,rock collapses,landslides,and rock bursts.True triaxial compression tests were conducted to analyze the fracture reactivation process under two different orientations of σ_(2),i.e.σ_(2) parallel to the fracture plane(Scheme 2)and σ_(2) cutting through the fracture plane(Scheme 3),under varying σ_(3) from 10 MPa to 40 MPa.The peak or fracture reactivation strength,deformation,failure mode,and post-peak mechanical behavior of intact(Scheme 1)and pre-fractured(Schemes 2 and 3)specimens were also compared.Results show that for intact specimens,the stress remains nearly constant in the residual sliding stage with no stick-slip,and the newly formed fracture surface only propagates along the σ_(2) direction when σ_(3) ranges from 10 MPa to 30 MPa,while it extends along both σ_(2) and σ_(3) directions when σ_(3) increases to 40 MPa;for the pre-fractured specimens,the fractures are usually reactivated under all the σ_(3) levels in Scheme 2,but fracture reactivation only occurs when σ_(3) is greater than 25 MPa in Scheme 3,below which new faulting traversing the original macro fracture occurs.In all the test schemes,both ε_(2) and ε_(3) experience an accumulative process of elongation,after which an abrupt change occurs at the point of the final failure;the degree of this change is dependent on the orientation of the new faulting or the slip direction of the original fracture,and it is generally more than 10 times larger in the slip direction of the original fracture than in the non-slip direction.Besides,the differential stress(peak stress)required for reactivation and the post-peak stress drop increase with increasing σ_(3).Post-peak stress drop and residual strength in Scheme 3 are generally greater than those in Scheme 2 at the same σ_(3) value.Our study clearly shows that intermediate principal stress orientation not only affects the fracture reactivation strength but also influences the slip deformation and failure modes.These new findings facilitate the mitigation of dynamic geological hazards associated with fracture and fault slip. 展开更多
关键词 True triaxial Fracture reactivation intermediate principal stress orientation Minimum principal stress levels Computed tomography
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True triaxial unloading test on the mechanical behaviors of sandstone:Effects of the intermediate principal stress and structural plane 被引量:1
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作者 Fan Feng Zhiwei Xie +3 位作者 Shaojie Chen Diyuan Li Siyu Peng Tong Zhang 《Journal of Rock Mechanics and Geotechnical Engineering》 2025年第4期2208-2226,共19页
A series of true triaxial unloading tests are conducted on sandstone specimens with a single structural plane to investigate their mechanical behaviors and failure characteristics under different in situ stress states... A series of true triaxial unloading tests are conducted on sandstone specimens with a single structural plane to investigate their mechanical behaviors and failure characteristics under different in situ stress states.The experimental results indicate that the dip angle of structural plane(θ)and the intermediate principal stress(σ2)have an important influence on the peak strength,cracking mode,and rockburst severity.The peak strength exhibits a first increase and then decrease as a function ofσ2 for a constantθ.However,whenσ2 is constant,the maximum peak strength is obtained atθof 90°,and the minimum peak strength is obtained atθof 30°or 45°.For the case of an inclined structural plane,the crack type at the tips of structural plane transforms from a mix of wing and anti-wing cracks to wing cracks with an increase inσ2,while the crack type around the tips of structural plane is always anti-wing cracks for the vertical structural plane,accompanied by a series of tensile cracks besides.The specimens with structural plane do not undergo slabbing failure regardless ofθ,and always exhibit composite tensile-shear failure whatever theσ2 value is.With an increase inσ2 andθ,the intensity of the rockburst is consistent with the tendency of the peak strength.By analyzing the relationship between the cohesion(c),internal friction angle(φ),andθin sandstone specimens,we incorporateθinto the true triaxial unloading strength criterion,and propose a modified linear Mogi-Coulomb criterion.Moreover,the crack propagation mechanism at the tips of structural plane,and closure degree of the structural plane under true triaxial unloading conditions are also discussed and summarized.This study provides theoretical guidance for stability assessment of surrounding rocks containing geological structures in deep complex stress environments. 展开更多
关键词 True triaxial unloading Dip angle of structural plane intermediate principal stress Mechanical behaviors Cracking modes Failure criterion
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Production of BTX through Catalytic Depolymerization of Lignin 被引量:1
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作者 范明慧 邓淑梅 +1 位作者 王铁军 李全新 《Chinese Journal of Chemical Physics》 SCIE CAS CSCD 2014年第2期221-226,I0004,共7页
Lignin is the only nature renewable resource which can provide large quantities of aromatic compounds. In the work, transformation of lignin into benzene, toluene, and xylenes (BTX) was investigated over the HZSM-5,... Lignin is the only nature renewable resource which can provide large quantities of aromatic compounds. In the work, transformation of lignin into benzene, toluene, and xylenes (BTX) was investigated over the HZSM-5, HY, and MCM-22 catalysts, and the HZSM-5 catalyst showed the highest carbon yield of BTX. The reaction condition, including temperature, the gas flow rate, and the catalyst/lignin ratio, was also investigated. The carbon yield of BTX reached about 25.3 C-mol% over HZSM-5 catalyst under T=550℃, f(N2)=300 cm^3/min, and catalyst/lignin ratio of 2. 展开更多
关键词 LIGNIN BENZENE TOLUENE XYLENES depolymerization
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Selective reduction of carbon dioxide to carbon monoxide over Au/CeO_2 catalyst and identification of reaction intermediate 被引量:2
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作者 朱晓兵 曲新 +4 位作者 李小松 刘景林 刘剑豪 朱斌 石川 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2016年第12期2053-2058,共6页
CO2 selective reduction to CO with H2 over a CeO2-supported nano-Au catalyst at atmospheric pres- sure was investigated. A high CO2 conversion, approaching the thermodynamic equilibrium value, and nearly 100% CO selec... CO2 selective reduction to CO with H2 over a CeO2-supported nano-Au catalyst at atmospheric pres- sure was investigated. A high CO2 conversion, approaching the thermodynamic equilibrium value, and nearly 100% CO selectivity were obtained. The surface formate intermediates generated during the reverse water-gas shift reaction at 400 ℃ were identified using in situ diffuse-reflectance infra- red Fourier-transform spectroscopy. The formate consumption to give CO and H20, determined using mass spectrometry, indicated that the reaction proceeded via an associative formate mecha- nism; this contributes to the high Au/CeO2 catalytic activity at low temperatures. 展开更多
关键词 CO2 reductionAu/CeO2 catalystCarbon monoxide Formate intermediate In situ DRIFT spectroscopy
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Non-planar vibration characteristics and buckling behaviors of two fluid-conveying pipes coupled with an intermediate spring
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作者 Dali WANG Tianli JIANG +1 位作者 Huliang DAI Lin WANG 《Applied Mathematics and Mechanics(English Edition)》 2025年第10期1829-1850,共22页
This study investigates the dynamical behavior of two parallel fluid-conveying pipes by developing a non-planar dynamical model of the two pipes coupled with an intermediate spring. A systematic analysis is conducted ... This study investigates the dynamical behavior of two parallel fluid-conveying pipes by developing a non-planar dynamical model of the two pipes coupled with an intermediate spring. A systematic analysis is conducted to evaluate the effects of spring parameters on the non-planar vibration characteristics and buckling behaviors of the coupled system. The nonlinear governing equations are derived with Hamilton's principle,subsequently discretized through Galerkin's method, and finally numerically solved by the Runge-Kutta algorithm. Based on the linearized equations, an eigenvalue analysis is performed to obtain the coupled frequencies, modal shapes, and critical flow velocities for buckling instability. Quantitative assessments further elucidate the effects of the spring position and stiffness coefficient on the coupled frequencies and critical flow velocities.Nonlinear dynamic analyses reveal the evolution of buckling patterns and bifurcation behaviors between the lateral displacements of the two pipes and the flow velocity. Numerical results indicate that the intermediate spring increases the susceptibility to buckling instability in the out-of-plane direction compared with the in-plane direction. Furthermore, synchronized lateral displacements emerge in both pipes when the flow velocity of one pipe exceeds the critical threshold. This work is expected to provide a theoretical foundation for the stability assessment and vibration analysis in coupled fluid-conveying pipe systems. 展开更多
关键词 coupled fluid-conveying pipe system intermediate spring non-planar vibration buckling behavior
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Increased tumor necrosis factor-receptor superfamily plasma levels are associated with early renal or retinal involvement in intermediate hyperglycemia
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作者 Sebastian Mas-Fontao Esther Civantos +7 位作者 Nisa Boukichou-Abdelkader Juan Antonio Moreno Carmen Gomez-Guerrero M Isabel López Gálvez Jaakko Tuomilehto Marcus Lind Rafael Gabriel Jesús Egido 《World Journal of Diabetes》 2025年第9期139-154,共16页
BACKGROUND Diabetes and its associated microvascular complications,such as nephropathy and retinopathy,significantly impact global health.These complications often begin in the prediabetic stage,emphasizing the import... BACKGROUND Diabetes and its associated microvascular complications,such as nephropathy and retinopathy,significantly impact global health.These complications often begin in the prediabetic stage,emphasizing the importance of early detection and intervention.Inflammatory pathways are key contributors to these conditions,and recent research has identified members of the tumor necrosis factor(TNF)receptor superfamily as potential biomarkers.However,their association with renal and retinal dysfunction in individuals with intermediate hyperglycemia(IH)remains underexplored.The Early Prevention of Diabetes Complications(ePREDICE)trial provides a valuable cohort to investigate these associations and improve risk assessment strategies.AIM To identify inflammatory biomarkers associated with early renal and retinal dysfunction in individuals with IH.Specifically,we evaluate the diagnostic and prognostic potential of TNF receptor superfamily members[TNF receptor 1(TNF-R1),TNF receptor 2(TNF-R2)],T-cell immunoglobulin and mucin domain 3(TIM-3)/HAVCR2,galectin-3,and interleukin-6(IL-6)in detecting kidney dysfunction and retinopathy in this high-risk population.By understanding their roles,we seek to enhance early screening methods and inform personalized intervention strategies.METHODS A cross-sectional analysis of 967 individuals with IH from the ePREDICE trial was conducted.Participants underwent comprehensive anthropometric and biochemical assessments.Key inflammatory biomarkers,including TNF-R1,TNF-R2,TIM-3/HAVCR2,galectin-3,and IL-6,were quantified using immunoassays.Renal function was assessed using estimated glomerular filtration rate(eGFR)and albuminuria,while retinopathy was evaluated through fundoscopic examination.Statistical analyses included adjusted mean comparisons,correlation studies,and receiver operating characteristic curve analysis to assess biomarker diagnostic accuracy.RESULTS TNF-R1,TNF-R2,and TIM-3/HAVCR2 were significantly associated with reduced filtration function(eGFR<60 mL/minute/1.73 m^(2))and albuminuria,with area under the curve(AUC)values between 0.815 and 0.845.TIM-3/HAVCR2 emerged as the strongest predictor of retinopathy(AUC=0.737).Strong correlations(r>0.75)were observed among TNF-R1,TNF-R2,and TIM-3/HAVCR2,suggesting a coordinated role in inflammatory pathways.CONCLUSION Our findings highlight the potential of TNF receptor superfamily members as biomarkers for early-stage renal and retinal complications in individuals with IH.Their integration into clinical screening protocols could facilitate earlier detection,improving patient stratification and personalized management strategies.Further longitudinal studies are necessary to validate their predictive value and potential for guiding therapeutic interventions in IH and early diabetes management. 展开更多
关键词 Biomarkers Microvascular complications intermediate hyperglycemia Renal function Tumor necrosis factor receptor
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Simultaneous enhancement of tensile strength and electrical conductivity of drawn Cu–20 wt.% Fe wire through intermediate annealing
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作者 Fei Yang Can-hui Wu +7 位作者 Yuan-fang Wang Rui-feng Li Feng-jian Shi Wen-yi Huo Li-ming Dong Jun Zhou Yan-xin Qiao Feng Fang 《Journal of Iron and Steel Research International》 2025年第10期3410-3425,共16页
The deformation of Cu–20 wt.%Fe alloy wires leads to a significant improvement in mechanical properties and a decrease in electrical conductivity.Simultaneous improvements in strength and conductivity were achieved b... The deformation of Cu–20 wt.%Fe alloy wires leads to a significant improvement in mechanical properties and a decrease in electrical conductivity.Simultaneous improvements in strength and conductivity were achieved by intermediate annealing of drawn Cu–20 wt.%Fe wires.As the annealing temperature increased,the strength of Cu–20 wt.%Fe alloy wire decreased monotonically,but the electrical conductivity first increased and then decreased,reaching its peak value after annealing at 500℃.The decrease in strength is related to dislocation recovery and static recrystallization of Cu and Fe phases,and the increase in electrical conductivity mainly results from the aging precipitation of solid solution Fe.After annealing at 500℃,there was no obvious recrystallization of Cu phase,and many of the nano-Fe particles precipitated from Cu matrix.An annealing temperature of 600℃ induced the recrystallization of Cu matrix and an increase in Fe solid solubility,resulting in a decrease in strength and electrical conductivity.Subsequently,the wires annealed at 500℃ were drawn to 2 mm.Compared with those of the continuously drawn Cu–20 wt.%Fe alloy wires,the deformation ability,strength,and electrical conductivity of Cu–20 wt.%Fe alloy wires subjected to intermediate annealing treatment are significantly greater.This is mainly related to the sufficient precipitation of Fe in Cu matrix and the strengthening of refined Fe fibers parallel to the drawing direction. 展开更多
关键词 Cu-Fe alloy wire Drawing deformation intermediate annealing Electrical conductivity Mechanical property
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Enhancement of Li^(+)Transport Through Intermediate Phase in High‑Content Inorganic Composite Quasi‑Solid‑State Electrolytes
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作者 Haoyang Yuan Wenjun Lin +3 位作者 Changhao Tian Mihaela Buga Tao Huang Aishui Yu 《Nano-Micro Letters》 2025年第11期630-645,共16页
Quasi-solid-state electrolytes,which integrate the safety characteristics of inorganic materials,the flexibility of polymers,and the high ionic conductivity of liquid electrolytes,represent a transitional solution for... Quasi-solid-state electrolytes,which integrate the safety characteristics of inorganic materials,the flexibility of polymers,and the high ionic conductivity of liquid electrolytes,represent a transitional solution for high-energy-density lithium batteries.However,the mechanisms by which inorganic fillers enhance multiphase interfacial conduction remain inadequately understood.In this work,we synthesized composite quasi-solid-state electrolytes with high inorganic content to investigate interfacial phenomena and achieve enhanced electrode interface stability.Li_(1.3)Al_(0.3)Ti_(1.7)(PO_(4))_(3)particles,through surface anion anchoring,improve Li^(+)transference numbers and facilitate partial dissociation of solvated Li^(+)structures,resulting in superior ion transport kinetics that achieve an ionic conductivity of 0.51 mS cm^(−1)at room temperature.The high mass fraction of inorganic components additionally promotes the formation of more stable interfacial layers,enabling lithium-symmetric cells to operate without short-circuiting for 6000 h at 0.1 mA cm^(−2).Furthermore,this system demonstrates exceptional stability in 5 V-class lithium metal full cells,maintaining 80.5%capacity retention over 200 cycles at 0.5C.These findings guide the role of inorganic interfaces in composite electrolytes and demonstrate their potential for advancing high-voltage lithium battery technology. 展开更多
关键词 Quasi-solid-state electrolytes Lithium metal anode intermediate phase Na-superionic-conductors 5 V-class cathode
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National survey of radiotherapy and androgen deprivation therapy strategies with PSMA-PET/CT integration in intermediate-risk prostate cancer:TROD 09-007 study
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作者 Aysenur Elmali Birhan Demirhan +3 位作者 Caglayan Selenge Beduk Esen Ozan Cem Guler Pervin Hurmuz Cem Onal 《The Canadian Journal of Urology》 2025年第4期243-254,共12页
Background:Intermediate-risk prostate cancer(IR-PC)represents a heterogeneous group requiring nuanced treatment approaches,and recent advancements in radiotherapy(RT),androgen deprivation therapy(ADT),and prostatespec... Background:Intermediate-risk prostate cancer(IR-PC)represents a heterogeneous group requiring nuanced treatment approaches,and recent advancements in radiotherapy(RT),androgen deprivation therapy(ADT),and prostatespecific membrane antigen positron emission tomography(PSMA-PET/CT)imaging have prompted growing interest in personalized,risk-adapted management strategies.This study by the Turkish Society for Radiation Oncology aims to examine radiation oncologists’practices in managing IR-PC,focusing on RT and imaging modalities to identify trends for personalized treatments.Methods:A cross-sectional survey was conducted among Turkish radiation oncologists treating at least 50 prostate cancer(PC)cases annually.The 22-item questionnaire covered IR-PC management aspects such as risk stratification,imaging preferences,androgen deprivation therapy(ADT)use and duration,RT techniques,and treatment combinations.Anonymous responses were analyzed using descriptive statistics.Results:Thirty radiation oncologists participated,57%with over 20 years of experience.The median annual number of PC cases treated was 130.For risk stratification,43% followed the National Comprehensive Cancer Network(NCCN)guidelines,while 30%used the D’Amico classification.Imaging preferences revealed 47% favored PSMA-PET/CT.External beam RT was universally preferred,with 60% adopting ultra-hypofractionation.ADT was used by 97%,with 73% recommending it for unfavorable IR-PC cases.Short-term ADT(4–6 months)was the standard,administered concurrently with RT by 57%.Cardiovascular status influenced decisions for 97% of respondents,while 37% also considered patient age,preferences,and sexual health.Conclusions:This national survey demonstrates a shift toward personalized care in intermediate-risk prostate cancer in Turkey,marked by selective PSMA-PET/CT use,tailored ADT,and evolving radiotherapy practices.The findings underscore the importance of multidisciplinary collaboration—particularly between urologists and radiation oncologists—to optimize imaging integration and treatment outcomes. 展开更多
关键词 prostate cancer intermediate risk RADIOTHERAPY androgen deprivation therapy prostatespecific membrane antigen positron emission tomography
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