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Novel open-framework chalcogenide photocatalysts:Cobalt cocatalyst valence state modulating critical charge transfer pathways towards high-efficiency hydrogen evolution
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作者 Haiyan Yin Abdusalam Ablez +4 位作者 Zhuangzhuang Wang Weian Li Yanqi Wang Qianqian Hu Xiaoying Huang 《Chinese Journal of Structural Chemistry》 2025年第4期44-55,共12页
Negatively charged open-framework metal sulfides(NOSs),taking advantages of the characteristics of excellent visible light absorption,easily exchanged cations,and abundant active sites,hold significant promise as high... Negatively charged open-framework metal sulfides(NOSs),taking advantages of the characteristics of excellent visible light absorption,easily exchanged cations,and abundant active sites,hold significant promise as highly efficient photocatalysts for hydrogen evolution.However,their applications in photocatalytic hydrogen evolution(PHE)are infrequently documented and the corresponding photocatalytic mechanism has not yet been explored.Herein,we excavated a novel NOS photocatalyst of(Me_(2)NH_(2))_(6)In_(10)S_(18)(MIS)with a three-dimensional(3D)structure,and successfully incorporated divalent Co(Ⅱ)and metal Co(0)into its cavities via the convenient cation exchange-assisted approach to regulate the critical steps of photocatalytic reactions.As the introduced Co(0)allows for more efficient light utilization and adroitly surficial hydrogen desorption,and meanwhile acts as the‘electron pump’for rapid charge transfer,Co(0)-modified MIS delivers a surprising PHE activity in the initial stage of photocatalysis.With the prolonging of illumination,metal Co(0)gradually escapes from MIS framework,resulting in the decline of PHE performance.By stark contrast,the incorporated Co(Ⅱ)can establish a strong interaction with MIS framework,and simultaneously capture photogenerated electrons from MIS to produce Co(0),which constructs a stable photocatalytic system as well as provides additional channels for spatially separating photogenerated carriers.Thus,Co(Ⅱ)-modified MIS exhibits a robust and highly stable PHE activity of~4944μmol/g/h during the long-term photocatalytic reactions,surpassing most of the previously reported In–S framework photocatalysts.This work represents a breakthrough in the study of PHE performance and mechanism of NOS-based photocatalysts,and sheds light on the design of vip confined NOS-based photocatalysts towards high-efficiency solar-to-chemical energy conversion. 展开更多
关键词 OPEN-FRAMEWORK Metal sulfide Ion exchange Cobalt cocatalyst valence state Charge transfer Photocatalytic hydrogen evolution
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Valence electron matching law for MXene-based single-atom catalysts
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作者 Pei Song Yuhang Zhou +9 位作者 Zishan Luo Hang Zhang Xi Sun Sen Lu Zepeng Jia Hong Cui Weizhi Tian Rong Feng Lingxia Jin Hongkuan Yuan 《Journal of Energy Chemistry》 2025年第2期641-650,I0013,共11页
Single-atom catalysts(SACs)have attracted considerable interest in the fields of energy and environmental science due to their adjustable catalytic activity.In this study,we investigated the matching of valence electr... Single-atom catalysts(SACs)have attracted considerable interest in the fields of energy and environmental science due to their adjustable catalytic activity.In this study,we investigated the matching of valence electron numbers between single atoms and adsorbed intermediates(O,N,C,and H)in MXene-anchored SACs(M-Ti_(2)C/M-Ti_(2)CO_(2)).The density functional theory results demonstrated that the sum of the valence electron number(VM)of the interface-doped metal and the valence electron number(VA)of the adsorbed intermediates in M-Ti_(2)C followed the 10-valence electron matching law.Furthermore,based on the 10-valence electron matching law,we deduced that the sum of the valence electron number(k)and VMfor the molecular adsorption intermediate interactions in M-Ti_(2)CO_(2)adhered to the 11-valence electron matching law.Electrostatic repulsion between the interface electrons in M-Ti_(2)CO_(2)and H_(2)O weakened the adsorption of intermediates,Furthermore,we applied the 11-valence electron matching law to guide the design of catalysts for nitrogen reduction reaction,specifically for N_(2)→NNH conversion,in the MTi_(2)CO_(2)structure.The sure independence screening and sparsifying operator algorithm was used to fit a simple three-dimensional descriptor of the adsorbate(R_(2)up to 0.970)for catalyst design.Our study introduced a valence electron matching principle between doped metals(single atoms)and adsorbed intermediates(atomic and molecular)for MXene-based catalysts,providing new insights into the design of high-performance SACs. 展开更多
关键词 Density functional theory Nitrogen reduction reaction Sure independence screening and sparsifying operator valence electron matching law
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Morphology and valence state evolution of Cu:Unraveling the impact on nitric oxide electroreduction 被引量:2
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作者 Ting Sun Fengyu Gao +4 位作者 Ya Wang Honghong Yi Qingjun Yu Shunzheng Zhao Xiaolong Tang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第4期276-286,共11页
Ammonia(NH3)serves as a critical component in the fertilizer industry and fume gas denitrification.However,the conventional NH3production process,namely the Haber-Bosch process,leads to considerable energy consumption... Ammonia(NH3)serves as a critical component in the fertilizer industry and fume gas denitrification.However,the conventional NH3production process,namely the Haber-Bosch process,leads to considerable energy consumption and waste gas emissions.To address this,electrocatalytic nitric oxide reduction reaction(NORR)has emerged as a promising strategy to bridge NH3consumption to NH3production,harnessing renewable electricity for a sustainable future.Copper(Cu)stands out as a prominent electrocatalyst for NO reduction,given its exceptional NH3yield and selectivity.However,a crucial aspect that remains insufficiently explored is the effects of morphology and valence states of Cu on the NORR performance.In this investigation,we synthesized CuO nanowires(CuO-NF)and Cu nanocubes(Cu-NF)as cathodes through an in situ growth method.Remarkably,CuO-NF exhibited an impressive NH3yield of 0.50±0.02 mg cm^(-2)h^(-1)at-0.6 V vs.reversible hydrogen electrode(RHE)with faradaic efficiency of29,68%±1,35%,surpassing that of Cu-NF(0.17±0.01 mg cm^(-2)h^(-1),16.18%±1.40%).Throughout the electroreduction process,secondary cubes were generated on the CuO-NF surface,preserving their nanosheet cluster morphology,sustained by an abundant supply of subsurface oxygen(s-O)even after an extended duration of 10 h,until s-O depletion ensued.Conversely,Cu-NF exhibited inadequate s-O content,leading to rapid crystal collapse within the same timeframe.The distinctive current-potential relationship,akin to a volcano-type curve,was attributed to distinct NO hydrogenation mechanisms.Further Tafel analysis revealed the exchange current density(i0)and standard heterogeneous rate constant(k0)for CuO-NF,yielding 3.44×10^(-6)A cm^(-2)and 3.77×10^(-6)cm^(-2)s^(-1)when NORR was driven by overpotentials.These findings revealed the potential of CuO-NF for NO reduction and provided insights into the intricate interplay between crystal morphology,valence states,and electrochemical performance. 展开更多
关键词 NORR Ammonia Synthesis COPPER MORPHOLOGY valence States Mechanism
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Valence electron structures dependences of structural stability and properties of REX_(3)(RE=rare earth;X=In,Tl)and RE(In,Co)_(3) alloys
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作者 Boyang Li Yongquan Guo +2 位作者 Yi-Chen Feng Xinze Wang Wei Liu 《Chinese Physics B》 SCIE EI CAS CSCD 2024年第11期331-339,共9页
Intermetallic compounds REIn_(3)(RE=rare earth)have attracted much attention due to their unique characteristics:crystal field effect,Kondo effect,superconductivity,heavy fermion,and antiferromagnetism,and their cobal... Intermetallic compounds REIn_(3)(RE=rare earth)have attracted much attention due to their unique characteristics:crystal field effect,Kondo effect,superconductivity,heavy fermion,and antiferromagnetism,and their cobalt diluted alloys exhibit the ferromagnetic half-metallic characteristics at room temperature.In this study,an empirical electron theory(EET)is employed to investigate systemically the valence electronic structure,the thermal and magnetic properties of REX_(3) and their cobalt diluted alloys for revealing the mechanism of physical properties.The calculated bond length,melting point,and magnetic moment match the experimental ones very well.The study reveals that structural stability and physical properties of REX_(3) and their cobalt dilute alloys are strongly related to their valence electron structures.It is suggested that the structural stability and cohesive energy depend upon the covalent electron,the melting point is modulated by covalent electron pair,and the magnetic moment is originated from 3d magnetic electron.The ferromagnetic characteristics of Co-diluted REIn3 alloys is originated from the introduction of strong ferromagnetic Co atom,but,a competition is caused between the electron transition from valence electron to magnetic electron on d orbit and its reversal electron transformation with increasing the content of cobalt,which results in the formations of diluted magnetic Gd(In,Co)_(3) alloy with minor amount of cobalt and strong magnetic Nd(In,Co)_(3) alloy with doping more Co atoms. 展开更多
关键词 REX_(3) cobalt dilute alloy valence electron structures empirical electron theory MOMENT
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Valence Bands Convergence in p-Type CoSb_(3) through Electronegative Fluorine Filling
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作者 黄写格 李家良 +5 位作者 马浩钦 李昌隆 刘天乐 段波 翟鹏程 李国栋 《Chinese Physics Letters》 SCIE EI CAS CSCD 2024年第7期87-94,共8页
Band convergence is considered to be a strategy with clear benefits for thermoelectric performance,generally favoring the co-optimization of conductivity and Seebeck coefficients,and the conventional means include ele... Band convergence is considered to be a strategy with clear benefits for thermoelectric performance,generally favoring the co-optimization of conductivity and Seebeck coefficients,and the conventional means include elemental filling to regulate the band.However,the influence of the most electronegative fluorine on the CoSb_(3) band remains unclear.We carry out density-functional-theory calculations and show that the valence band maximum gradually shifts downward with the increase of fluorine filling,lastly the valence band maximum converges to the highly degenerated secondary valence bands in fluorine-filled skutterudites. 展开更多
关键词 valence CONVERGENCE BANDS
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Enhanced anomalous Hall effect in kagome magnet YbMn_(6)Sn_(6)with intermediate-valence ytterbium
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作者 李龙飞 迟晟玮 +3 位作者 马文龙 郭凯臻 徐刚 贾爽 《Chinese Physics B》 SCIE EI CAS CSCD 2024年第5期43-50,共8页
We report on the magnetization and anomalous Hall effect(AHE)in the high-quality single crystals of the kagome magnet YbMn_(6)Sn_(6),where the spins of the Mn atoms in the kagome lattice order ferromagnetically and th... We report on the magnetization and anomalous Hall effect(AHE)in the high-quality single crystals of the kagome magnet YbMn_(6)Sn_(6),where the spins of the Mn atoms in the kagome lattice order ferromagnetically and the intermediate-valence Yb atoms are nonmagnetic.The intrinsic mechanism plays a crucial role in the AHE,leading to an enhanced anomalous Hall conductivity(AHC)compared with the other rare-earth RMn_(6)Sn_(6)compounds.Our band structure calculation reveals a strong hybridization between the 4f electrons of Yb and conduction electrons. 展开更多
关键词 anomalous Hall effect kagome magnet intermediate valence
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Net valence analysis of iris recognition technology-based FinTech
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作者 Mutaz M.Al-Debei Omar Hujran Ahmad Samed Al-Adwan 《Financial Innovation》 2024年第1期2339-2385,共47页
Iris recognition technology(IRT)-based authentication is a biometric financial technology(FinTech)application used to automate user recognition and verification.In addition to being a controversial technology with var... Iris recognition technology(IRT)-based authentication is a biometric financial technology(FinTech)application used to automate user recognition and verification.In addition to being a controversial technology with various facilitators and inhibitors,the adoption of IRT-based FinTech is driven by contextual factors,such as customer perceptions,deployed biometric technology,and financial transaction settings.Due to its controversial and contextual properties,analyzing IRT-based FinTech acceptance is challenging.This study uses a net valence framework to investigate the salient positive and negative factors influencing the intention to use IRT-based FinTech in automated teller machines(ATMs)in Jordan.This study is pertinent because there is a dearth of research on IRT-based FinTech in the relevant literature;most previous research has taken purely engineering and technical approaches.Furthermore,despite considerable investments by banks and other financial institutions in this FinTech,target user adoption is minimal,and only 6% of Jordan’s ATM transactions are currently IRT-enabled.This study employs mixed methods.In the first qualitative study,17 Jordanian customers were interviewed regarding the benefits and risks of IRT-based FinTech in ATMs.Content analyses determined the most important concepts or themes.The advantages include financial security,convenience,and FinTech-enabled hygiene,whereas the concerns include performance,financial,privacy,and physical risks.The research model is constructed based on the qualitative study and theoretical underpinnings,wherein 631 Jordanian bank customers with active ATM accounts were surveyed to validate the research model.The findings indicate that IRT-based FinTech usage in ATMs is proportional to its perceived value.In descending order of effect,financial security,FinTech-enabled hygiene,and convenience benefits positively impact perceived value.Privacy,financial,and physical risks have negative impacts on perceived value,whereas performance risk has no effect.This study contributes to the relatively untapped domain of biometric technology in information systems,with important theoretical and practical implications. 展开更多
关键词 Iris recognition technology(IRT) FinTech Biometric technology Net valence Perceived value Adoption intention JORDAN
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Equalized Electronegativity Based on the Valence Electrons and Its Application 被引量:2
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作者 武亚新 曹晨忠 袁华 《Chinese Journal of Chemical Physics》 SCIE CAS CSCD 2011年第1期31-39,I0003,共10页
We take the contribution of all valence electrons into consideration and propose a new valence electrons equilibration method to calculate the equalized electronegativity including molecular electronegativity, group e... We take the contribution of all valence electrons into consideration and propose a new valence electrons equilibration method to calculate the equalized electronegativity including molecular electronegativity, group electronegativity, and atomic charge. The ionization potential of alkanes and mono-substituted alkanes, the chemical shift of 1H NMR, and the gas phase proton affinity of aliphatic amines, alcohols, and ethers were estimated. All the expressions have good correlations. Moreover, the Sanderson method and Bratsch method were modified on the basis of the valence electrons equilibration theory. The modified Sanderson method and modified Bratsch method are more effective than their original methods to estimate these properties. 展开更多
关键词 Electronegativity equalization valence electrons equilibration method Molecular electronegativity Group electronegativity Atomic charge
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STUDY ON DEGRADATION OF LDPE CATALYZED BY MULTI-VALENCE METALLIC ORGANIC COMPOUNDS AT COMPOST TEMPERATURE
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作者 于九皋 陈崧哲 《Transactions of Tianjin University》 EI CAS 2001年第4期290-293,共4页
The catalytic effects of the organic compounds of iron,tin and manganese on the degradation of low density polyethylene (LDPE) at compost temperature are discussed.A series of samples were aged in a simulating compost... The catalytic effects of the organic compounds of iron,tin and manganese on the degradation of low density polyethylene (LDPE) at compost temperature are discussed.A series of samples were aged in a simulating compost environment.The mechanical properties,viscosity average molecular weight (M η) of PE and hydroperoxide (POOH) concentration in the samples were measured.FT IR and DSC were also applied to characterize some samples.It was shown that the above mentioned metallic organic compounds can catalyze the degradation of LDPE efficiently.After 2 months aging,all samples with catalysts became fragile and the M η of the material decreased dramatically.Furthermore,the concentration of carbonyl and the degree of crystallinity of the material increased with the aging time. 展开更多
关键词 polyethylene multi valence metallic organic compound COMPOST DEGRADATION HYDROPEROXIDE
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Valence states, impurities and electrocrystallization behaviors during molten salt electrorefining for preparation of high-purity titanium powder from sponge titanium 被引量:11
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作者 翁启刚 李瑞迪 +2 位作者 袁铁锤 李健 贺跃辉 《Transactions of Nonferrous Metals Society of China》 SCIE EI CAS CSCD 2014年第2期553-560,共8页
High-purity titanium powder was prepared by molten salt electrorefining from sponge titanium in NaCl-KCl-TiClx salts. The titanium valence, purity and electrocrystallization during electrolysis process were studied. T... High-purity titanium powder was prepared by molten salt electrorefining from sponge titanium in NaCl-KCl-TiClx salts. The titanium valence, purity and electrocrystallization during electrolysis process were studied. The XPS analysis showed that the titanium valences are mainly +4, +3 and +2 at the earlier, medium and later stages of electrolysis, respectively. During the electrolysis process, the contents of impurities Si, Cr, Mn, Al vary little, and the contents of impurities Fe, Cu, Ni decrease markedly, while the contents of impurities O, N, H increase obviously. The residual impurities are usually distributed in small tunnel of dendritic crystals. Enhancing the electrolysis temperature and prolonging the electrolysis time can increase the titanium particle size. The TEM analysis showed that the electrodeposited titanium is not a single crystal, but contains many nanostructured grains and subgrains, with grain size of 100-500 nm. The electrolysis mechanisms were also discussed. 展开更多
关键词 molten salt electrolysis high-purity titanium powder valence ELECTROCRYSTALLIZATION
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V2O5 Nanospheres with Mixed Vanadium Valences as High Electrochemically Active Aqueous Zinc-Ion Battery Cathode 被引量:18
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作者 Fei Liu Zixian Chen +5 位作者 Guozhao Fang Ziqing Wang Yangsheng Cai Boya Tang Jiang Zhou Shuquan Liang 《Nano-Micro Letters》 SCIE EI CAS CSCD 2019年第2期98-108,共11页
AV4+-V2O5 cathode with mixed vanadium valences was prepared via a novel synthetic method using VOOH as the precursor,and its zinc-ion storage performance was evaluated.The products are hollow spheres consisting of nan... AV4+-V2O5 cathode with mixed vanadium valences was prepared via a novel synthetic method using VOOH as the precursor,and its zinc-ion storage performance was evaluated.The products are hollow spheres consisting of nanoflakes.The V4+-V2O5 cathode exhibits a prominent cycling performance,with a specific capacity of 140 mAhg-1 after 1000 cycles at 10 A g.1,and an excellent rate capability.The good electrochemical performance is attributed to the presence of V4+,which leads to higher electrochemical activity,lower polarization,faster ion diffusion,and higher electrical conductivity than V2O5 without V4+.This engineering strategy of valence state manipulation may pave the way for designing high-performance cathodes for elucidating advanced battery chemistry. 展开更多
关键词 V2O5 MIXED valences Hollow sphere Long-cycle-life AQUEOUS zinc-ion BATTERY
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High valence metals engineering strategies of Fe/Co/Ni-based catalysts for boosted OER electrocatalysis 被引量:14
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作者 Lu Li Xianjun Cao +6 位作者 Juanjuan Huo Junpeng Qu Weihua Chen Chuntai Liu Yufei Zhao Hao Liu Guoxiu Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第1期195-213,I0006,共20页
Electrocatalysis for the oxygen evolution reactions(OER)has attracted much attention due to its important role in water splitting and rechargeable metal-air batteries.Therefore,designing highly efficient and low-cost ... Electrocatalysis for the oxygen evolution reactions(OER)has attracted much attention due to its important role in water splitting and rechargeable metal-air batteries.Therefore,designing highly efficient and low-cost catalysts for OER process is essential as the conventional catalysts still rely on precious metals.Transition metal-based compounds have been widely investigated as active OER catalysts,and renewed interest in the high valence metals engineered compounds has been achieved for superior catalytic activity and stability.However,an in-depth understanding of the construction strategies and induced effects for the high valence metals engineered catalysts is still lacking and desired.In this review,we have summarized the construction strategies of high valence metals as dopants or formed heterostructures with the iron/cobalt/nickel(Fe/Co/Ni)-based catalysts.Then the induced effects on Fe/Co/Ni-based catalysts by incorporating high valence metals,e.g.,accelerating the surface reconstruction,forming amorphous structure,generating vacancies/defects,and acting as stabilizers,are highlighted.The impacts of high valence metals on OER performance are elucidated based on different elements,including molybdenum(Mo),tungsten(W),cerium(Ce),vanadium(V),chromium(Cr),manganese(Mn),niobium(Nb),zirconium(Zr).The correlations of construction strategies,induced effects,catalytic activity and OER reaction pathways are elaborated.Finally,the remaining challenges for further enhancements of OER performance induced by high valence metals are presented. 展开更多
关键词 High valence metals Construction strategies Induced effect Oxygen evolution reactions
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Effects of 4f Electron Characteristics and Alternation Valence of Rare Earths on Photosynthesis: Regulating Distribution of Energy and Activities of Spinach Chloroplast 被引量:7
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作者 刘晓晴 苏明玉 +3 位作者 刘超 张易 司文会 洪法水 《Journal of Rare Earths》 SCIE EI CAS CSCD 2007年第4期495-501,共7页
Chloroplasts were isolated from spinach treated with taCl3, CeCl3, and NdCl3. Because of owning 4f electron characteristics and alternation valence, Ce treatment presented the highest enhancement in light absorption, ... Chloroplasts were isolated from spinach treated with taCl3, CeCl3, and NdCl3. Because of owning 4f electron characteristics and alternation valence, Ce treatment presented the highest enhancement in light absorption, energy transfer from LHC Ⅱ to PS Ⅱ, excitation energy distribution from PS Ⅰ to PS Ⅱ, and fluorescence quantum yield around 680 nm. Compared with Ce treatment, Nd treatment resulted in relatively lower enhancement in these physiological indices, as Nd did not have alternation valence. La treatment presented the lowest enhancement, as La did not have either 4f electron or alternation valence. The increase in activities of whole chain electron transport, PS ⅡDCPIP photoreduction, and oxygen evolution of chloroplasts was of the following order: Ce〉Nd 〉La〉 control. However, the photoreduction activities of spinach PS I almost did not change with La, Ce, or Nd treatments. The results suggested that 4f electron characteristics and alternation valence of rare earths had a close relationship with photosynthesis improvement. 展开更多
关键词 4f electron characteristic and alternation valence SPINACH CHLOROPLAST energy transfer and distribution photochemical activity rare earths
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ASTUDY OF VALENCE OF YTTRIUM IN Y_2O_3 Mo CATHODE 被引量:20
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作者 J.S.Wang1,2) ,M.L.Zhou2) ,J.X.Zhang2) ,Z.R.Nie2) T.Y.Zuo2) and G.J.Zhang2) 1) State Key Laboratory of Materials Chemistry and Applications,Peking University ,Beijing 100871 ,China2) Schoolof Materials Science and Engineering ,Beijing Polytechnic Univers 《Acta Metallurgica Sinica(English Letters)》 SCIE EI CAS CSCD 1999年第4期602-606,共5页
The valenceofelementyttrium of Y2 O3 Mocathode materialhasbeenstudied by usingther mal weight analysis, X ray diffraction analysis, Scanning electron microscopy and X rayphotoelectronspectrum . It hasbeen proved... The valenceofelementyttrium of Y2 O3 Mocathode materialhasbeenstudied by usingther mal weight analysis, X ray diffraction analysis, Scanning electron microscopy and X rayphotoelectronspectrum . It hasbeen provedthatyttrium oxidecan bereduced by molybdenum carbide. Thereaction between powdered Y2 O3 and Mo2 Ccan happen at 1173 , and Y2 O3may bereduced to metallicyttrium . Afterthepowder mixtureof Y2 O3 and Mo2 Cwasheat treated at1873 K, Yttrium existsin two kinds of chemicalstate- yttrium of zero valence and yttrium ofthreevalences. 展开更多
关键词 valence yttrium Y2 O3 Mo cathode
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New insights into FeS/persulfate system for tetracycline elimination:Iron valence,homogeneous-heterogeneous reactions and degradation pathways 被引量:5
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作者 Jinhong Fan Ying Cai +1 位作者 Shihao Shen Lin Gu 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2022年第2期48-58,共11页
In this study,complete tetracycline(TTC)and above 50%of total organic carbon(TOC)were removed by Fe S/PS after 30 min under optimized conditions.Although free radicals and high-valent iron ions were identified to gene... In this study,complete tetracycline(TTC)and above 50%of total organic carbon(TOC)were removed by Fe S/PS after 30 min under optimized conditions.Although free radicals and high-valent iron ions were identified to generate in the process,the apparent similarity between intermediate products of Fe S/PS,Fe/PS,and UV/PS systems demonstrated that the degradation of TTC was due to sulfate radicals(SO_(4)·^(-))and hydroxyl radicals(·OH).Based on the reaction between free radicals and organic matter,we speculated that TTC in the Fe S/PS system was decomposed and mineralized by dehydration,dehydrogenation,hydroxyl addition,demethylation,substitution,E-transfer,and ring-opening.Furthermore,a new understanding of Fe S-mediated PS activation based on stoichiometry and kinetic analysis showed that there were both homogeneous and heterogeneous reactions that occurred in the entire progress.However,due to the effect of p H on the dissolution of iron ions,the homogeneous reaction became the principal process with iron ions concentration exceeding 1.35 mg/L.This work provides a theoretical basis for the study of the degradation of TTC-containing wastewater by the iron-based advanced oxidation process. 展开更多
关键词 TETRACYCLINE Persulfate activation Iron valence Homogeneous-heterogeneous reactions Degradation pathways
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In-situ optimizing the valence configuration of vanadium sites in NiV-LDH nanosheet arrays for enhanced hydrogen evolution reaction 被引量:5
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作者 Danyang He Liyun Cao +6 位作者 Jianfeng Huang Koji Kajiyoshi Jianpeng Wu Changcong Wang Qianqian Liu Dan Yang Liangliang Feng 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2020年第8期263-271,I0010,共10页
Developing the highly active, cost-effective, environmental-friendly, and ultra-stable nonprecious electrocatalysts for hydrogen evolution reaction(HER) is distinctly indispensable for the large-scale practical applic... Developing the highly active, cost-effective, environmental-friendly, and ultra-stable nonprecious electrocatalysts for hydrogen evolution reaction(HER) is distinctly indispensable for the large-scale practical applications of hydrolytic hydrogen production. Herein, we report the synthesis of well-integrated electrode, NiV layered double hydroxide nanosheet array grown in-situ on porous nickel foam(abbreviated as in-NiV-LDH/NF) via the facile one-step hydrothermal route. Interestingly, the valence configuration of vanadium(V) sites in such NiV-LDH are well dominated by the innovative use of NF as the reducing regulator, achieving the reassembled in-NiV-LDH/NF with a high proportion of trivalent V ions(V3+), and then an enhanced intrinsic electrocatalytic HER activity. The HER testing results show that the in-NiVLDH/NF drives the current densities of 10 and 100 mA cm-2 at extremely low overpotentials of 114 and 245 mV without iR-compensation respectively, even outperforms commercial 20 wt% Pt/C at the large current density of over 80 mA cm-2 in alkaline media, as well as gives robust catalytic durability of at least 100 h in both alkaline and neutral media. More importantly, this work provides a fresh perspective for designing bimetal(oxy) hydroxides electrocatalysts with efficient hydrogen generation. 展开更多
关键词 NiV-LDH V sites valence configuration Stability Hydrogen evolution reaction
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Structural evolution and superconductivity tuned by valence electron concentration in the Nb-Mo-Re-Ru-Rh high-entropy alloys 被引量:6
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作者 Bin Liu Jifeng Wu +5 位作者 Yanwei Cui Qjnqing Zhu Guorui Xiao Siqi Wu Guang-han Cao Zhi Ren 《Journal of Materials Science & Technology》 SCIE EI CAS CSCD 2021年第26期11-17,共7页
The crystal structure and physical properties of Nb_(25)Mo_(5+x)Re_(35)Ru_(25-x)Rh_(10)(0≤x≤10)and Nb_(5)Mo_(35-y)Re_(15+y)Ru_(35)Rh_(10)(0≤y≤15)high-entropy alloys(HEAs)have been studied by X-ray diffraction,elec... The crystal structure and physical properties of Nb_(25)Mo_(5+x)Re_(35)Ru_(25-x)Rh_(10)(0≤x≤10)and Nb_(5)Mo_(35-y)Re_(15+y)Ru_(35)Rh_(10)(0≤y≤15)high-entropy alloys(HEAs)have been studied by X-ray diffraction,electrical resistivity,magnetic susceptibility,and specific heat measurements.The results show that the former HEAs with valence electron concentration(VEC)values of 6.7-6.9 crystallize in a noncentrosymmetric cubicα-Mn structure,while the latter ones with VEC values of 7.1-7.25 adopt a centrosymmetric hexagonal close-packed(hcp)structure.Despite different structures,both series of HEAs are found to be bulk superconductors with a full energy gap,and the superconducting transition temperature Tc tends to decrease with the increase of VEC.Nevertheless,the Tc values of the hcp-type HEAs are higher than those of theα-Mn-type ones,likely due to a stronger electron phonon coupling.Furthermore,we show that VEC and electronegativity difference are two key parameters to control the stability ofα-Mn and hcp-type HEAs.These results not only are helpful for the design of such HEAs,but also represent the first realization of structurally different HEA superconductors without changing the constituent elements. 展开更多
关键词 High-entropy alloys Hcp toα-Mn structural evolution Superconducting properties valence electron concentration Electronegativity difference
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Boosting the cell performance of the SiO_(x)@C anode material via rational design of a Si-valence gradient 被引量:6
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作者 Jianming Tao Zerui Yan +3 位作者 Jiangshao Yang Jiaxin Li Yingbin Lin Zhigao Huang 《Carbon Energy》 SCIE CAS 2022年第2期129-141,共13页
Relieving the stress or strain associated with volume change is highly desirable for high-performance SiOx anodes in terms of stable solid electrolyte interphase(SEI)-film growth.Herein,a Si-valence gradient is optimi... Relieving the stress or strain associated with volume change is highly desirable for high-performance SiOx anodes in terms of stable solid electrolyte interphase(SEI)-film growth.Herein,a Si-valence gradient is optimized in SiOx composites to circumvent the large volume strain accompanied by lithium insertion/extraction.SiO_(x)@C annealed at 850℃ has a gentle Si-valence gradient along the radial direction and excellent electrochemical performances,delivering a high capacity of 506.9 mAh g^(−1) at 1.0 A g^(−1) with a high Coulombic efficiency of~99.8%over 400 cycles.Combined with the theoretical prediction,the obtained results indicate that the gentle Si-valence gradient in SiO_(x)@C is useful for suppressing plastic deformation and maintaining the inner connection integrity within the SiO_(x)@C particle.Moreover,a gentle Si-valence gradient is expected to form a stress gradient and affect the distribution of dangling bonds,resulting in local stress relief during the lithiation/delithiation process and enhanced Li-ion kinetic diffusion.Furthermore,the lowest interfacial stress variation ensures a stable SEI film at the interface and consequently increases cycling stability.Therefore,rational design of a Si-valence gradient in SiOx can provide further insights into achieving high-performance SiOx anodes with large-scale production. 展开更多
关键词 lithium-ion battery SEI film growth SiO_(x)@C stress valence gradient
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High valence state of Ni and Mo synergism in NiS_(2);MoS_(2)hetero-nanorods catalyst with layered surface structure for urea electrocatalysis 被引量:4
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作者 Shuli Wang Linyu Zhao +3 位作者 Jiaxin Li Xinlong Tian Xiang Wu Ligang Feng 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第3期483-492,I0013,共11页
High valence state species are significant in the energy-relevant electrochemical oxidation reactions.Herein,the high active state of Ni^(3+)formation induced by Mo^(6+)and their efficient synergism in NiS_(2)-MoS_(2)... High valence state species are significant in the energy-relevant electrochemical oxidation reactions.Herein,the high active state of Ni^(3+)formation induced by Mo^(6+)and their efficient synergism in NiS_(2)-MoS_(2)hetero-nanorods powder catalyst with the rough layered structure are demonstrated,as proof of concept,for the urea-assisted water electrolysis.This catalyst can be derived from the sulfidation of NiMoO_(4) nanorods that can realize individual metal sulfides sufficiently mixing at a domain size in the nanoscale which creates lots of active sites and nanointerfaces.The high valence state of Mo^(6+)and Ni^(3+)formation and increased conductive phase of 1 T MoS_(2)in the hetero-nanorods compared to the counterpart pure phases are revealed by spectral study and microscopic analysis;high electrochemical surface area and active site exposure are found due to the nano-interface formation and layered rough nanosheets over the surface of nanorods.They show much higher catalytic performance than their pure phases for urea oxidation,including high catalytic activity,stability,charge transfer ability and catalytic kinetics resulting from more active Ni^(3+)species formation and electronic synergism of high valence metals.Transformation of 1 T MoS_(2)to Mo^(6+)and increased amount of Mo^(6+)and Ni^(3+)after stability test indicate their involvement and synergism for the catalysis reaction.The current work offers a novel understanding of the synergistic effect based on the high valence state synergism for heterogeneous catalysts in electrocatalysis. 展开更多
关键词 Hetero-nanorods High valence state Urea oxidation NiS_(2) MoS_(2)
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Microstructure,phase composition and wear resistance of low valence electron concentration Al_(x)CoCrFeNiSi high-entropy alloys prepared by vacuum arc melting 被引量:3
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作者 Bing-qian Jin Nan-nan Zhang +1 位作者 Yue Zhang De-yuan Li 《Journal of Iron and Steel Research International》 SCIE EI CAS CSCD 2021年第2期181-189,共9页
The low valence electron concentration(VEC)Al_(x)CoCrFeNiSi(x=0.5,1.0,1.5 and 2.0)high-entropy alloys(HEAs)were designed by the fundamental properties of the constituent elements and prepared by vacuum arc melting met... The low valence electron concentration(VEC)Al_(x)CoCrFeNiSi(x=0.5,1.0,1.5 and 2.0)high-entropy alloys(HEAs)were designed by the fundamental properties of the constituent elements and prepared by vacuum arc melting method.The effects of Al addition on the crystal structure and microstructure were investigated.The microhardness and wear property were also researched.The results showed that the microstructure transformed from dendritic crystal to equiaxed crystal.It was found that FCC phase gradually decreased with the increasing Al content and disappeared until in a composition of 1.0 in Al_(x)CoCrFeNiSi HEAs.Little FCC phase was found with continuously adding Al,while the phase fraction of BCC increased from 85.0% to 91.8%,and VEC decreased from 7.00 to 6.14.The microhardness was increased gradually from 598 up to 909 HV with addition of Al from 0.5 to 2.0.It was the same of the compressive strength results,which improved from 1200 to 1920 MPa.The wear coefficient and mass loss were in line with mechanical properties evolution,which was attributed to the microstructure transformation into equiaxed crystal and the increase in BCC phase. 展开更多
关键词 High-entropy alloy valence electron concentration MICROSTRUCTURE Phase assemblage Wear resistance
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