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Engineering oxygen vacancies on Tb-doped ceria supported Pt catalyst for hydrogen production through steam reforming of long-chain hydrocarbon fuels
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作者 Zhourong Xiao Changxuan Zhang +5 位作者 Peng Li Desong Wang Xiangwen Zhang Li Wang Jijun Zou Guozhu Li 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第4期181-192,共12页
Steam reforming of long-chain hydrocarbon fuels for hydrogen production has received great attention for thermal management of the hypersonic vehicle and fuel-cell application.In this work,Pt catalysts supported on Ce... Steam reforming of long-chain hydrocarbon fuels for hydrogen production has received great attention for thermal management of the hypersonic vehicle and fuel-cell application.In this work,Pt catalysts supported on CeO_(2)and Tb-doped CeO_(2)were prepared by a precipitation method.The physical structure and chemical properties of the as-prepared catalysts were characterized by powder X-ray diffraction,scanning electron microscopy,transmission electron microscopy,Raman spectroscopy,H_(2)temperature programmed reduction,and X-ray photoelectron spectroscopy.The results show that Tb-doped CeO_(2)supported Pt possesses abundant surface oxygen vacancies,good inhibition of ceria sintering,and strong metal-support interaction compared with CeO_(2)supported Pt.The catalytic performance of hydrogen production via steam reforming of long-chain hydrocarbon fuels(n-dodecane)was tested.Compared with 2Pt/CeO_(2),2Pt/Ce_(0.9)Tb_(0.1)O_(2),and 2Pt/Ce_(0.5)Tb_(0.5)O_(2),the 2Pt/Ce_(0.7)Tb_(0.3)O_(2)has higher activity and stability for hydrogen production,on which the conversion of n-dodecane was maintained at about 53.2%after 600 min reaction under 700℃at liquid space velocity of 9 ml·g^(-1)·h^(-1).2Pt/CeO_(2)rapidly deactivated,the conversion of n-dodecane was reduced to only 41.6%after 600 min. 展开更多
关键词 Steam reforming N-DODECANE hydrogen production Pt-based catalyst oxygen vacancy CeO_(2)
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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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Defect engineering and Ni promoter synergistically accelerating electron transfer to Ru^(0) sites in UiO-66(Ce) for dicyclopentadiene hydrogenation under mild condition
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作者 Rushuo Li Tao Ban +6 位作者 Danfeng Zhao Jing Lin Zhiyuan Liu Linmeng Wang Xiubing Huang Zhiping Tao Ge Wang 《Nano Research》 SCIE EI CSCD 2024年第11期9550-9563,共14页
Olefin hydrogenation under mild condition is crucial and challenging for industrial applications. Herein, defective UiO-66(Ce) was constructed by using cyanuric acid as the molecular etching “scissors” and further t... Olefin hydrogenation under mild condition is crucial and challenging for industrial applications. Herein, defective UiO-66(Ce) was constructed by using cyanuric acid as the molecular etching “scissors” and further to synthesize heterogeneous catalyst with highly dispersed RuNi nanoparticles (Ru1Ni1.5@UiO-66(Ce)-12 h). The construction of Ce-O-Ru/Ni heterogeneous interfaces and Ni–Ru bonds provide electron transfer channels from Ce-oxo clusters and Ni species to Ru species. Furthermore, the microenvironment and electronic structure of Ru0 active sites were synergistically regulated by adjusting the content of metal-organic frameworks (MOFs) defects and Ni promoter, thereby enhancing the adsorption and activation ability of H–H and C=C bonds. Therefore, Ru1Ni1.5@UiO-66(Ce)-12 h achieved dicyclopentadiene saturated hydrogenation (100% conversion) to tetrahydrodicyclopentadiene (∼ 100% selectivity) under mild condition (35℃, 1 MPa) with only 25 min. Meanwhile, the sample exhibited excellent structural stability after 6 cycles test. This study provides a promising strategy for the rational design of remarkable noble metal-based catalysts for practical applications. 展开更多
关键词 metal-organic frameworks defect engineering Ni promoter electron-rich Ru^(0)active sites dicyclopentadiene hydrogenation
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Facet Engineering of Advanced Electrocatalysts Toward Hydrogen/Oxygen Evolution Reactions 被引量:10
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作者 Changshui Wang Qian Zhang +7 位作者 Bing Yan Bo You Jiaojiao Zheng Li Feng Chunmei Zhang Shaohua Jiang Wei Chen Shuijian He 《Nano-Micro Letters》 SCIE EI CAS CSCD 2023年第4期97-137,共41页
The electrocatalytic water splitting technology can generate highpurity hydrogen without emitting carbon dioxide,which is in favor of relieving environmental pollution and energy crisis and achieving carbon neutrality... The electrocatalytic water splitting technology can generate highpurity hydrogen without emitting carbon dioxide,which is in favor of relieving environmental pollution and energy crisis and achieving carbon neutrality.Electrocatalysts can effectively reduce the reaction energy barrier and increase the reaction efficiency.Facet engineering is considered as a promising strategy in controlling the ratio of desired crystal planes on the surface.Owing to the anisotropy,crystal planes with different orientations usually feature facet-dependent physical and chemical properties,leading to differences in the adsorption energies of oxygen or hydrogen intermediates,and thus exhibit varied electrocatalytic activity toward hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In this review,a brief introduction of the basic concepts,fundamental understanding of the reaction mechanisms as well as key evaluating parameters for both HER and OER are provided.The formation mechanisms of the crystal facets are comprehensively overviewed aiming to give scientific theory guides to realize dominant crystal planes.Subsequently,three strategies of selective capping agent,selective etching agent,and coordination modulation to tune crystal planes are comprehensively summarized.Then,we present an overview of significant contributions of facet-engineered catalysts toward HER,OER,and overall water splitting.In particular,we highlight that density functional theory calculations play an indispensable role in unveiling the structure–activity correlation between the crystal plane and catalytic activity.Finally,the remaining challenges in facet-engineered catalysts for HER and OER are provided and future prospects for designing advanced facet-engineered electrocatalysts are discussed. 展开更多
关键词 Crystal facet engineering ANISOTROPY oxygen evolution reaction hydrogen evolution reaction Theoretical simulations
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Boosting Hydrogen Storage Performance of MgH_(2) by Oxygen Vacancy-Rich H-V_(2)O_(5) Nanosheet as an Excited H-Pump 被引量:2
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作者 Li Ren Yinghui Li +4 位作者 Zi Li Xi Lin Chong Lu Wenjiang Ding Jianxin Zou 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第8期398-416,共19页
MgH_(2) is a promising high-capacity solid-state hydrogen storage material,while its application is greatly hindered by the high desorption temperature and sluggish kinetics.Herein,intertwined 2D oxygen vacancy-rich V... MgH_(2) is a promising high-capacity solid-state hydrogen storage material,while its application is greatly hindered by the high desorption temperature and sluggish kinetics.Herein,intertwined 2D oxygen vacancy-rich V_(2)O_(5) nanosheets(H-V_(2)O_(5))are specifically designed and used as catalysts to improve the hydrogen storage properties of MgH_(2).The as-prepared MgH_(2)-H-V_(2)O_(5) composites exhibit low desorption temperatures(Tonset=185℃)with a hydrogen capacity of 6.54 wt%,fast kinetics(Ea=84.55±1.37 kJ mol^(-1) H_(2) for desorption),and long cycling stability.Impressively,hydrogen absorption can be achieved at a temperature as low as 30℃ with a capacity of 2.38 wt%within 60 min.Moreover,the composites maintain a capacity retention rate of~99%after 100 cycles at 275℃.Experimental studies and theoretical calculations demonstrate that the in-situ formed VH_(2)/V catalysts,unique 2D structure of H-V_(2)O_(5) nanosheets,and abundant oxygen vacancies positively contribute to the improved hydrogen sorption properties.Notably,the existence of oxygen vacancies plays a double role,which could not only directly accelerate the hydrogen ab/de-sorption rate of MgH_(2),but also indirectly affect the activity of the catalytic phase VH_(2)/V,thereby further boosting the hydrogen storage performance of MgH_(2).This work highlights an oxygen vacancy excited“hydrogen pump”effect of VH_(2)/V on the hydrogen sorption of Mg/MgH_(2).The strategy developed here may pave a new way toward the development of oxygen vacancy-rich transition metal oxides catalyzed hydride systems. 展开更多
关键词 hydrogen storage MgH_(2) V_(2)O_(5)nanosheets oxygen vacancies VH_(2)
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Enhancing hydrogen evolution and oxidation kinetics through oxygen insertion into nickel lattice
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作者 Wanli Liang Xiyu Gong +9 位作者 Jinchang Xu Zixuan Dan Fanyan Xie Hulei Yu Hao-Fan Wang Yanshuo Jin Hongjuan Wang Yonghai Cao Hui Meng Hao Yu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第8期529-539,I0012,共12页
Nickel-based materials,including metallic Ni and Ni oxide,have been widely studied in the exploration of non-precious-metal hydrogen electrocatalysts,but neither pure Ni nor NiO is ideal for the hydrogen evolution rea... Nickel-based materials,including metallic Ni and Ni oxide,have been widely studied in the exploration of non-precious-metal hydrogen electrocatalysts,but neither pure Ni nor NiO is ideal for the hydrogen evolution reaction(HER)and hydrogen oxidation reaction(HOR).In this paper,an oxygen insertion strategy was applied on nickel to regulate its hydrogen electrocatalytic performance,and the oxygen-inserted nickel catalyst was successfully obtained with the assistance of tungsten dioxide support(denoted as O-Ni/WO_(2)).The partial insertion of oxygen in Ni maintains the face-centered cubic arrangement of Ni atoms,simultaneously expanding the lattice and increasing the lattice spacing.Consequently,the adsorption strength of^(*)H and^(*)OH on Ni is optimized,thus resulting in superior electrocatalytic performance of0-Ni/WO_(2)in alkaline HER/HOR.The Tafel slope of O-Ni/WO_(2)@NF for HER is 56 mV dec^(-1),and the kinetic current density of O-Ni/WO_(2)for HOR reaches 4.85 mA cm^(-2),which is ahead of most currently reported catalysts.Our proposed strategy of inserting an appropriate amount of anions into the metal lattice could provide more possibilities for the design of high-performance catalysts. 展开更多
关键词 hydrogen evolution hydrogen oxidation NICKEL oxygen insertion Adsorption free energy
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Unveiling the chemistry behind the electrolytic production of hydrogen peroxide by oxygenated carbon
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作者 Pan Xiang Kunshang Yang +6 位作者 Qihao Yang Yang Gao Wenwen Xu Zhiyi Lu Liang Chen Zhiming Wang Ziqi Tian 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第9期49-58,共10页
Oxygenated carbon materials exhibit outstanding electrocatalytic performance in the production of hydrogen peroxide(H2O2)through a two-electron oxygen reduction reaction.The nature of the active functional group and u... Oxygenated carbon materials exhibit outstanding electrocatalytic performance in the production of hydrogen peroxide(H2O2)through a two-electron oxygen reduction reaction.The nature of the active functional group and underlying reaction mechanism,however,remain unclear.Here,a comprehensive workflow was established to identify the active sites from the numerous possible structures.The common hydroxyl group at the notched edge demonstrates a key role in the two-electron process.The local chemical environment weakens the binding of OOH intermediate to substrate while enhancing interaction with solution,thereby promoting the H_(2)O_(2)production.With increasing pH,the intramolecular hydrogen bond between OOH intermediate and hydroxyl decreases,facilitating OOH desorption.Furthermore,the rise in selectivity with increasing potential stems from the suppression of the four-electron process.The active site was further validated through experiments.Guided by theoretical understanding,optimal performance was achieved with high selectivity(>95%)and current density(2.06 mA/cm^(2))in experiment. 展开更多
关键词 First-principles calculation oxygen reductionreaction hydrogen peroxide production Fixed-potential method oxygenated carbon materials
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Biomimetic Erythrocyte-Like Particles from Microfluidic Electrospray for Tissue Engineering
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作者 Zhiqiang Luo Lijun Cai +2 位作者 Hanxu Chen Guopu Chen Yuanjin Zhao 《Engineering》 SCIE EI CAS CSCD 2024年第9期78-86,共9页
Microparticles have demonstrated value for regenerative medicine.Attempts in this field tend to focus on the development of intelligent multifunctional microparticles for tissue regeneration.Here,inspired by erythrocy... Microparticles have demonstrated value for regenerative medicine.Attempts in this field tend to focus on the development of intelligent multifunctional microparticles for tissue regeneration.Here,inspired by erythrocytes-associated self-repairing process in damaged tissue,we present novel biomimetic erythrocyte-like microparticles(ELMPs).These ELMPs,which are composed of extracellular matrix-like hybrid hydrogels and the functional additives of black phosphorus,hemoglobin,and growth factors(GFs),are generated by using a microfluidic electrospray.As the resultant ELMPs have the capacity for oxygen delivery and near-infrared-responsive release of both GFs and oxygen,they would have excellent biocompatibility and multifunctional performance when serving as microscaffolds for cell adhesion,stimulating angiogenesis,and adjusting the release profile of cargoes.Based on these features,we demonstrate that the ELMPs can stably overlap to fill a wound and realize controllable cargo release to achieve the desired curative effect of tissue regeneration.Thus,we consider our biomimetic ELMPs with discoid morphology and cargo-delivery capacity to be ideal for tissue engineering. 展开更多
关键词 Biomimetics ERYTHROCYTE Tissue engineering MICROFLUIDICS ELECTROSPRAY oxygen delivery
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Defect-engineered two-dimensional transition metal dichalcogenides towards electrocatalytic hydrogen evolution reaction 被引量:5
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作者 Hang Su Xiaodong Pan +2 位作者 Suqin Li Hao Zhang Ruqiang Zou 《Carbon Energy》 SCIE CSCD 2023年第6期21-44,共24页
Recently,two-dimensional transition metal dichalcogenides(TMDs)demonstrated their great potential as cost-effective catalysts in hydrogen evolution reaction.Herein,we systematically summarize the existing defect engin... Recently,two-dimensional transition metal dichalcogenides(TMDs)demonstrated their great potential as cost-effective catalysts in hydrogen evolution reaction.Herein,we systematically summarize the existing defect engineering strategies,including intrinsic defects(atomic vacancy and active edges)and extrinsic defects(metal doping,nonmetal doping,and hybrid doping),which have been utilized to obtain advanced TMD-based electrocatalysts.Based on theoretical simulations and experimental results,the electronic structure,intermediate adsorption/desorption energies and possible catalytic mechanisms are thoroughly discussed.Particular emphasis is given to the intrinsic relationship between various types of defects and electrocatalytic properties.Furthermore,current opportunities and challenges for mechanical investigations and applications of defective TMD-based catalysts are presented.The aim herein is to reveal the respective properties of various defective TMD catalysts and provide valuable insights for fabricating high-efficiency TMD-based electrocatalysts. 展开更多
关键词 defect engineering ELECTROCATALYSTS hydrogen evolution reaction(HER) transition metal dichalcogenides
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Defect Engineering and Carbon Supporting to Achieve Ni‑Doped CoP_(3) with High Catalytic Activities for Overall Water Splitting
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作者 Daowei Zha Ruoxing Wang +5 位作者 Shijun Tian Zhong‑Jie Jiang Zejun Xu Chu Qin Xiaoning Tian Zhongqing Jiang 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第11期569-584,共16页
This work reports the use of defect engineering and carbon supporting to achieve metal-doped phosphides with high activities and stabilities for the hydrogen evolution reaction(HER)and the oxygen evolution reaction(OE... This work reports the use of defect engineering and carbon supporting to achieve metal-doped phosphides with high activities and stabilities for the hydrogen evolution reaction(HER)and the oxygen evolution reaction(OER)in alkaline media.Specifically,the nitrogen-doped carbon nanofiber-supported Ni-doped CoP_(3) with rich P defects(Pv·)on the carbon cloth(p-NiCoP/NCFs@CC)is synthesized through a plasma-assisted phosphorization method.The p-NiCoP/NCFs@CC is an efficient and stable catalyst for the HER and the OER.It only needs overpotentials of 107 and 306 mV to drive 100 mA cm^(-2) for the HER and the OER,respectively.Its catalytic activities are higher than those of other catalysts reported recently.The high activities of the p-NiCoP/NCFs@CC mainly arise from its peculiar structural features.The density functional theory calculation indicates that the Pv·richness,the Ni doping,and the carbon supporting can optimize the adsorption of the H atoms at the catalyst surface and promote the strong electronic couplings between the carbon nanofiber-supported p-NiCoP with the surface oxide layer formed during the OER process.This gives the p-NiCoP/NCFs@CC with the high activities for the HER and the OER.When used in alkaline water electrolyzers,the p-NiCoP/NCFs@CC shows the superior activity and excellent stability for overall water splitting. 展开更多
关键词 PLASMA ELECTROCATALYSIS hydrogen evolution reaction oxygen evolution reaction Water splitting
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Pyrimidine-containing covalent organic frameworks for efficient photosynthesis of hydrogen peroxide via one-step two electron oxygen reduction process
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作者 Hongyu Chen Hao Zhang +1 位作者 Kai Chi Yan Zhao 《Nano Research》 SCIE EI CSCD 2024年第11期9498-9506,共9页
The photocatalytic oxygen reduction reaction (ORR), particularly the one-step two-electron (2e−) pathway, is a highly promising strategy for efficient and selective hydrogen peroxide (H_(2)O_(2)) synthesis. However, c... The photocatalytic oxygen reduction reaction (ORR), particularly the one-step two-electron (2e−) pathway, is a highly promising strategy for efficient and selective hydrogen peroxide (H_(2)O_(2)) synthesis. However, constructing efficient photocatalysts to achieve a one-step 2e− ORR process remains a significant challenge. Herein, we developed an efficient photocatalyst by incorporating pyrimidine units into benzotrithiophene-based covalent organic framework (BTT-MD-COF), enabling the photosynthesis of H_(2)O_(2) via the one-step 2e− ORR pathway with O_(2) and water. Under visible-light irradiation, BTT-MD-COF exhibited a high H_(2)O_(2) production rate of up to 5691.2 µmol·h^(−1)·g^(−1). Further experimental results and theoretical studies revealed that the introduction of pyrimidine units accelerates the separation of photoinduced electron–hole pairs and promotes Yeager-type O_(2) adsorption, which alters the two-step 2e− ORR process to the direct one-step 2e− process. This work offers a new avenue to create metal-free catalysts for efficient photosynthesis of H_(2)O_(2). 展开更多
关键词 covalent organic frameworks photocatalysis hydrogen peroxide oxygen reduction reaction pyrimidine units
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Defect engineering of ternary Cu-In-Se quantum dots for boosting photoelectrochemical hydrogen generation 被引量:2
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作者 Shi Li Sung-Mok Jung +10 位作者 Wookjin Chung Joo-Won Seo Hwapyong Kim Soo Ik Park Hyo Cheol Lee Ji Su Han Seung Beom Ha In Young Kim Su-Il In Jae-Yup Kim Jiwoong Yang 《Carbon Energy》 SCIE EI CAS CSCD 2023年第12期215-228,共14页
Heavy-metal-free ternary Cu–In–Se quantum dots(CISe QDs)are promising for solar fuel production because of their low toxicity,tunable band gap,and high light absorption coefficient.Although defects significantly aff... Heavy-metal-free ternary Cu–In–Se quantum dots(CISe QDs)are promising for solar fuel production because of their low toxicity,tunable band gap,and high light absorption coefficient.Although defects significantly affect the photophysical properties of QDs,the influence on photoelectrochemical hydrogen production is not well understood.Herein,we present the defect engineering of CISe QDs for efficient solar-energy conversion.Lewis acid–base reactions between metal halide–oleylamine complexes and oleylammonium selenocarbamate are modulated to achieve CISe QDs with the controlled amount of Cu vacancies without changing their morphology.Among them,CISe QDs with In/Cu=1.55 show the most outstanding photoelectrochemical hydrogen generation with excellent photocurrent density of up to 10.7 mA cm-2(at 0.6 VRHE),attributed to the suitable electronic band structures and enhanced carrier concentrations/lifetimes of the QDs.The proposed method,which can effectively control the defects in heavy-metal-free ternary QDs,offers a deeper understanding of the effects of the defects and provides a practical approach to enhance photoelectrochemical hydrogen generation. 展开更多
关键词 copper-indium-selenide defect engineering photoelectrochemical hydrogen generation quantum dots solar hydrogen
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Enhanced structural stability and durability in lithium-rich manganese-based oxide via surface double-coupling engineering
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作者 Jiayu Zhao Yuefeng Su +10 位作者 Jinyang Dong Xi Wang Yun Lu Ning Li Qing Huang Jianan Hao Yujia Wu Bin Zhang Qiongqiong Qi Feng Wu Lai Chen 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第11期274-283,共10页
Lithium-rich manganese-based oxides(LRMOs) exhibit high theoretical energy densities, making them a prominent class of cathode materials for lithium-ion batteries. However, the performance of these layered cathodes of... Lithium-rich manganese-based oxides(LRMOs) exhibit high theoretical energy densities, making them a prominent class of cathode materials for lithium-ion batteries. However, the performance of these layered cathodes often declines because of capacity fading during cycling. This decline is primarily attributed to anisotropic lattice strain and oxygen release from cathode surfaces. Given notable structural transformations, complex redox reactions, and detrimental interface side reactions in LRMOs, the development of a single modification approach that addresses bulk and surface issues is challenging. Therefore,this study introduces a surface double-coupling engineering strategy that mitigates bulk strain and reduces surface side reactions. The internal spinel-like phase coating layer, featuring threedimensional(3D) lithium-ion diffusion channels, effectively blocks oxygen release from the cathode surface and mitigates lattice strain. In addition, the external Li_(3)PO_(4) coating layer, noted for its superior corrosion resistance, enhances the interfacial lithium transport and inhibits the dissolution of surface transition metals. Notably, the spinel phase, as excellent interlayer, securely anchors Li_(3)PO_(4) to the bulk lattice and suppresses oxygen release from lattices. Consequently, these modifications considerably boost structural stability and durability, achieving an impressive capacity retention of 83.4% and a minimal voltage decay of 1.49 m V per cycle after 150 cycles at 1 C. These findings provide crucial mechanistic insights into the role of surface modifications and guide the development of high-capacity cathodes with enhanced cyclability. 展开更多
关键词 Lithium-ion battery Layered lithium-rich cathode Surface double-coupling engineering Lattice strain oxygen release
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Engineering Cu^(+)/CeZrO_(x) interfaces to promote CO_(2) hydrogenation to methanol 被引量:4
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作者 Jingpeng Zhang Xiaohang Sun +4 位作者 Congyi Wu Wenquan Hang Xu Hu Dawei Qiao Binhang Yan 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第2期45-53,I0002,共10页
Cu-based catalysts are widely employed for CO_(2) hydrogenation to methanol,which is expected as a promising process to achieving carbon neutrality.However,most Cu-based catalysts still suffer from low methanol yield ... Cu-based catalysts are widely employed for CO_(2) hydrogenation to methanol,which is expected as a promising process to achieving carbon neutrality.However,most Cu-based catalysts still suffer from low methanol yield with a passable CO_(2) conversion and lack insight into its reaction mechanism for guiding the design of catalysts.In this work,Cu^(+)/CeZrO_(x) interfaces are engineered by employing a series of ceria-zirconia solid solution catalysts with various Ce/Zr ratios,forming a Cu^(+)-O_(v)-Ce^(3+)structure where Cu^(+)atoms are bonded to the oxygen vacancies(O_(v))of ceria.Compared to Cu/CeO_(2) and Cu/ZrO_(2),the optimized catalyst(i.e.,Cu_(0.3)Ce_(0.3)Zr_(0.7))exhibits a much higher mass-specific methanol formation rate(192g_(MeOH)/kg_(cat)/h)at 240℃and 3 MPa.Through a series of in-situ and ex-situ characterization,it is revealed that oxygen vacancies in solid solutions can effectively assist the activation of CO_(2) and tune the electronic state of copper to promote the formation of Cu^(+)/CeZrO_(x) interfaces,which stabilizes the key*CO intermediate,inhibits its desorption and facilitates its further hydrogenation to methanol via the reverse watergas-shift(RWGS)+CO-Hydro pathway.Therefore,the concentration of*CO or the apparent Cu^(+)/(Cu^(+)+Cu^(0))ratio could be employed as a quantitative descriptor of the methanol formation rate.This work is expected to give a deep insight into the mechanism of metal/support interfaces in CO_(2) hydrogenation to methanol,offering an effective strategy to develop new catalysts with high performance. 展开更多
关键词 CO_(2)hydrogenation Methanol synthesis In-situ characterization Cu^(+)/CeZrO_(x)interfaces oxygen vacancies
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Origin of the Yueguang gold deposit in Xinhua, Hunan Province, South China: insights from fl uid inclusion and hydrogen–oxygen stable isotope analysis
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作者 Hongxin Fan Qiang Wang +2 位作者 Yulong Yang Yao Tang Hao Zou 《Acta Geochimica》 EI CAS CSCD 2024年第2期235-254,共20页
The Yueguang gold deposit is located in Fengjia,Xinhua County,Hunan Province,South China.It represents a recently discovered small-scale gold deposit situated in the southwestern region of the Jiangnan Orogenic Belt,w... The Yueguang gold deposit is located in Fengjia,Xinhua County,Hunan Province,South China.It represents a recently discovered small-scale gold deposit situated in the southwestern region of the Jiangnan Orogenic Belt,west of the Baimashan granitic batholith.In order to discern the characteristics of the ore-formingfluids,the underlying mineralization processes,and establish a foundation for the origin of the Yueguang gold depositfluid inclusion micro-thermometry,as well as quartz hydrogen and oxygen isotope analysis,have been carried out on samples obtained from various stages of mineralization.The hydrothermal miner-alization stages within the Yueguang gold deposit can be categorized into three stages:(i)the barren,pre-ore quartz-pyrite stage(Stage Ⅰ),the quartz-pyrite-gold stage(Stage Ⅱ),and the post-ore quartz-carbonate stage(Stage Ⅲ),with the second stage being the main mineralization stage.Thefluid inclusions identified in samples from the main min-eralization stage can predominantly be described with the NaCl–H_(2)O and CO_(2)–NaCl–H_(2)O systems.These inclusions display homogenization temperatures ranging from 158.8 to 334.9℃,and thefluid salinity ranges from 0.3%to 4.0%(wt.%NaCl equiv.).Laser Raman spectroscopy analysis of individual inclusions further reveals the presence of gas-phases such as CO_(2),CH_(4),and N_(2).Isotopic analysis indicatesδ^(18)Ofluid values ranging from 3.95 to 6.7‰ and δDH_(2)O values ranging from-71.9 to-55.7‰.These results indi-cate that the ore-formingfluid of the Yueguang gold deposit belongs to metamorphic hydrothermalfluids of middle-low temperature and low salinity.In the process of ore formation,gold is transported in the form of Au(HS)2-complexes,with gold deposition being driven byfluid immiscibility.Therefore,the Yueguang gold deposit is categorized as an orogenic gold deposit dominated by metamorphic hydrother-malfluid.It may become a new target for gold exploration in the Baimashan region,central Hunan Province. 展开更多
关键词 Hunan province Yueguang gold deposit Fluid inclusions hydrogenoxygen isotopes Laser Raman Fluid immiscibility Orogenic gold deposit
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Corrosion engineering on AlCoCrFeNi high-entropy alloys toward highly efficient electrocatalysts for the oxygen evolution of alkaline seawater 被引量:2
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作者 Zhibin Chen Kang Huang +4 位作者 Bowei Zhang Jiuyang Xia Junsheng Wu Zequn Zhang Yizhong Huang 《International Journal of Minerals,Metallurgy and Materials》 SCIE EI CAS CSCD 2023年第10期1922-1932,共11页
Seawater splitting is a prospective approach to yield renewable and sustainable hydrogen energy.Complex preparation processes and poor repeatability are currently considered to be an insuperable impediment to the prom... Seawater splitting is a prospective approach to yield renewable and sustainable hydrogen energy.Complex preparation processes and poor repeatability are currently considered to be an insuperable impediment to the promotion of the large-scale production and application of electrocatalysts.Avoiding the use of intricate instruments,corrosion engineering is an intriguing strategy to reduce the cost and presents considerable potential for electrodes with catalytic performance.An anode comprising quinary AlCoCrFeNi layered double hydroxides uniformly decorated on an AlCoCrFeNi high-entropy alloy is proposed in this paper via a one-step corrosion engineering method,which directly serves as a remarkably active catalyst for boosting the oxygen evolution reaction(OER)in alkaline seawater.Notably,the best-performing catalyst exhibited oxygen evolution reaction activity with overpotential values of 272.3 and 332 mV to achieve the current densities of 10 and100 mA·cm^(-2),respectively.The failure mechanism of the obtained catalyst was identified for advancing the development of multicomponent catalysts. 展开更多
关键词 corrosion engineering oxygen evolution reaction catalysts layered double hydroxides seawater splitting failure mechanism
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Increased Oxygen Vacancies in CuO-ZnO Snowflake-like Composites Drive the Hydrogenation of CO_(2) to Methanol
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作者 San Xiaoguang Wu Wanmeng +4 位作者 Zhang Lei Meng Dan Chang Xiangshuang Tan Jianen Qi Jian 《China Petroleum Processing & Petrochemical Technology》 SCIE CAS CSCD 2024年第2期22-33,共12页
Cu/ZnO is widely used in the hydrogenation of carbon dioxide (CO_(2)) to methanol (CH_(3)OH) to improve the lowconversion rate and selectivity generally observed. In this work, a series of In, Zr, Co, and Ni-doped CuO... Cu/ZnO is widely used in the hydrogenation of carbon dioxide (CO_(2)) to methanol (CH_(3)OH) to improve the lowconversion rate and selectivity generally observed. In this work, a series of In, Zr, Co, and Ni-doped CuO-ZnO catalysts wassynthesized via a hydrothermal method. By introducing a second metal element, the activity and dispersion of the activesites can be adjusted and the synergy between the metal and the carrier can be enhanced, forming an abundance of oxygenvacancies. Oxygen vacancies not only adsorb CO_(2) but also activate the intermediates in methanol synthesis, playing a keyrole in the entire reaction. Co3O4-CuO-ZnO had the best catalytic performance (a CO_(2) conversion rate of 9.17%;a CH_(3)OHselectivity of 92.77%). This study describes a typical strategy for multi-component doping to construct a catalyst with anabundance of oxygen vacancies, allowing more effective catalysis to synthesize CH_(3)OH from CO_(2). 展开更多
关键词 CuO-ZnO catalyst CO_(2)hydrogenation to CH_(3)OH doping oxygen vacancy SYNERGY
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Modulating surface oxygen species via facet engineering for efficient conversion of nitrate to ammonia 被引量:1
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作者 Wenye Zhong Zhiheng Gong +4 位作者 Zuyun He Nian Zhang Xiongwu Kang Xianwen Mao Yan Chen 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第3期211-221,I0007,共12页
Electrochemical reduction of nitrate,a common pollutant in aquatic environment,to valuable ammonia(NO3-RR) using renewably-sourced electricity has attracted widespread interests,with past efforts mainly focused on des... Electrochemical reduction of nitrate,a common pollutant in aquatic environment,to valuable ammonia(NO3-RR) using renewably-sourced electricity has attracted widespread interests,with past efforts mainly focused on designing electrocatalysts with high activity and selectivity.The detailed correlation between catalyst properties and NO3-RR kinetics,nevertheless,is still not fully understood.In this work,we modulate the surface oxygen species of Cu_(2)O via facet engineering,and systematically study the impact of these oxygen species on the NO_(3)^(-)RR activity.Combining advanced spectroscopic techniques,densi ty fu n ctional theory calculations and molecular dynamics simulations,we find that while oxygen vacancies on Cu_(2)O(111) surface promote the adsorption of reactants and reaction intermediates,hydroxyl groups effectively inhibit the side reaction of hydrogen evolution and facilitate the hydrogenation process of NO3-RR.These two effects work in concert to render Cu_(2)O(111) facet the highest NO3-RR activity relative to those from other facets.Our study provides critical insights into the synergistic effect of exposed facets and surface oxygen species on heterogeneous catalysis,and offers a generalizable,facet engineeringbased strategy for improving the performance of a variety of electrocatalysts important for renewable energy conversion. 展开更多
关键词 Facet engineering oxygen vacancy Hydroxyl group Electrochemical nitrate reduction AMMONIA
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Boosting the Performance Gain of Ru/C for Hydrogen Evolution Reaction Via Surface Engineering 被引量:1
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作者 Xiaobing Bao Yuzhuo Chen +3 位作者 Shanjun Mao Yong Wang Yong Yang Yutong Gong 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2023年第5期415-424,共10页
The surface properties of catalysts determine the intrinsic activity and adaptability.Ruthenium is regarded as a potential candidate to substitute platinum for water electrolysis due to the low cost and analogous elec... The surface properties of catalysts determine the intrinsic activity and adaptability.Ruthenium is regarded as a potential candidate to substitute platinum for water electrolysis due to the low cost and analogous electronic structures while it suffers from severe dissolution and stability problems.Herein,the modification of Ru/C with atomically dispersed cobalt atoms is achieved via a simple thermal doping method.The newly formed amorphous shell with Ru-Co sites on the Ru/C catalyst improved the hydrogen evolution reaction activity and stability significantly.Impressively,the obtained Co1Ru@Ru/CN_(x)catalyst exhibited an overpotential as low as 30 mV at 10 mA cm^(-2)in an alkaline medium,which is among the best HER catalysts reported so far.The oxygen oxophile Co prevents the fast oxidation and dissolution of Ru species,ensuring outstanding long-term durability up to 70 h.Theoretical calculations reveal that the Ru-Co coordination acts as a more active site for water dissociation than the Ru-Ru.Meanwhile,the"Ru-Co shell/Ru core"structures show high adaptability for the reaction conditions.This simple doping strategy offers prospects for scalable preparation of highly active electrocatalysts. 展开更多
关键词 high performance hydrogen evolution reaction ruthenium catalyst surface engineering
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Strain engineering and hydrogen effect for two-dimensional ferroelectricity in monolayer group-Ⅳmonochalcogenides MX(M=Sn,Ge;X=Se,Te,S)
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作者 Maurice Franck Kenmogne Ndjoko 郭必诞 +1 位作者 彭银辉 赵宇军 《Chinese Physics B》 SCIE EI CAS CSCD 2023年第3期396-401,共6页
Two-dimensional(2D)ferroelectric compounds are a special class of materials that meet the need for devices miniaturization,which can lead to a wide range of applications.Here,we investigate ferroelectric properties of... Two-dimensional(2D)ferroelectric compounds are a special class of materials that meet the need for devices miniaturization,which can lead to a wide range of applications.Here,we investigate ferroelectric properties of monolayer group-IV monochalcogenides MX(M=Sn,Ge;X=Se,Te,S)via strain engineering,and their effects with contaminated hydrogen are also discussed.GeSe,GeTe,and GeS do not go through transition up to the compressive strain of-5%,and consequently have good ferroelectric parameters for device applications that can be further improved by applying strain.According to the calculated ferroelectric properties and the band gaps of these materials,we find that their band gap can be adjusted by strain for excellent photovoltaic applications.In addition,we have determined the most stable hydrogen occupancy location in the monolayer SnS and SnTe.It reveals that H prefers to absorb on SnS and SnTe monolayers as molecules rather than atomic H.As a result,hydrogen molecules have little effect on the polarization and electronic structure of monolayer SnTe and SnS. 展开更多
关键词 two-dimensional material strain engineering ferroelectric photovoltaic materials hydrogen effect
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