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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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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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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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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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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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Co-Ru alloy nanoparticles decorated onto two-dimensional nitrogen doped carbon nanosheets towards hydrogen/oxygen evolution reaction and oxygen reduction reaction 被引量:2
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作者 Huizhen Wang Pengfei Yang +9 位作者 Xiaoyuan Sun Weiping Xiao Xinping Wang Minge Tian Guangrui Xu Zhenjiang Li Yubing Zhang Fusheng Liu Lei Wang Zexing Wu 《Journal of Energy Chemistry》 SCIE EI CSCD 2023年第12期286-294,I0008,共10页
Constructing highly-efficient electrocatalysts toward hydrogen evolution reaction(HER)/oxygen evolution reaction(OER)/oxygen reduction reaction(ORR)with excellent stability is quite important for the development of re... Constructing highly-efficient electrocatalysts toward hydrogen evolution reaction(HER)/oxygen evolution reaction(OER)/oxygen reduction reaction(ORR)with excellent stability is quite important for the development of renewable energy-related applications.Herein,Co-Ru based compounds supported on nitrogen doped two-dimensional(2D)carbon nanosheets(NCN)are developed via one step pyrolysis procedure(Co-Ru/NCN)for HER/ORR and following low-temperature oxidation process(Co-Ru@RuO_(x)/NCN)for OER.The specific 2D morphology guarantees abundant active sites exposure.Furthermore,the synergistic effects arising from the interaction between Co and Ru are crucial in enhancing the catalytic performance.Thus,the resulting Co-Ru/NCN shows remarkable electrocatalytic performance for HER(70 mV at 10 mA cm^(-2))in 1 M KOH and ORR(half-wave potential E_(1/2)=0.81 V)in 0.1 M KOH.Especially,the Co-Ru@RuO_(x)/NCN obtained by oxidation exhibits splendid OER performance in both acid(230 mV at 10 mA cm^(-2))and alkaline media(270 mV at 10 mA cm^(-2))coupled with excellent stability.Consequently,the fabricated two-electrode water-splitting device exhibits excellent performance in both acidic and alkaline environments.This research provides a promising avenue for the advancement of multifunctional nanomaterials. 展开更多
关键词 ELECTROCATALYST 2D Carbon nanosheet hydrogen/oxygen evolution reaction oxygen reduction reaction WATER-SPLITTING
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Adjusting oxygen vacancies in perovskite LaCoO_(3)by electrochemical activation to enhance the hydrogen evolution reaction activity in alkaline condition 被引量:1
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作者 Chengrong Wu Yan Sun +4 位作者 Xiaojian Wen Jia-Ye Zhang Liang Qiao Jun Cheng Kelvin H.L.Zhang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第1期226-232,I0006,共8页
Developing highly-active,earth-abundant non-precious-metal catalysts for hydrogen evolution reaction(HER)in alkaline solution would be beneficial to sustainable energy storage.Perovskite oxides are generally regarded ... Developing highly-active,earth-abundant non-precious-metal catalysts for hydrogen evolution reaction(HER)in alkaline solution would be beneficial to sustainable energy storage.Perovskite oxides are generally regarded as low-active HER catalysts,due to their inapposite hydrogen adsorption and water dissociation.Here,we report a detailed study on perovskite LaCoO_(3)epitaxial thin films as a model catalyst to significantly enhance the HER performance via an electrochemical activation process.As a result,the overpotential for the activation films to achieve a current density of 0.36 m A/cm^(2)is 238 m V,reduced by more than 200 m V in comparison with that of original samples.Structural characterization revealed the activation process dramatically increases the concentration of oxygen vacancies(Vo)on the surface of LaCoO_(3).We established the relationship between the electronic structure induced by Vo and the enhanced HER activity.Further theoretical calculations revealed that the Vo optimizes the hydrogen adsorption and dissociation of water on the surface of LaCoO_(3)thin films,thus improving the HER catalytic activity.This work may promote a deepened understanding of perovskite oxides for HER mechanism by Vo adjusting and a new avenue for designing highly active electrochemical catalysts in alkaline solution. 展开更多
关键词 hydrogen evolution reaction Perovskite oxides Activation process oxygen vacancies
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Oxygen‑Coordinated Single Mn Sites for Efficient Electrocatalytic Nitrate Reduction to Ammonia 被引量:2
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作者 Shengbo Zhang Yuankang Zha +8 位作者 Yixing Ye Ke Li Yue Lin Lirong Zheng Guozhong Wang Yunxia Zhang Huajie Yin Tongfei Shi Haimin Zhang 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第1期147-159,共13页
Electrocatalytic nitrate reduction reaction has attracted increasing attention due to its goal of low carbon emission and environmental protection.Here,we report an efficient NitRR catalyst composed of single Mn sites... Electrocatalytic nitrate reduction reaction has attracted increasing attention due to its goal of low carbon emission and environmental protection.Here,we report an efficient NitRR catalyst composed of single Mn sites with atomically dispersed oxygen(O)coordination on bacterial cellulose-converted graphitic carbon(Mn-O-C).Evidence of the atomically dispersed Mn-(O-C_(2))_(4)moieties embedding in the exposed basal plane of carbon surface is confirmed by X-ray absorption spectroscopy.As a result,the as-synthesized Mn-O-C catalyst exhibits superior NitRR activity with an NH_(3)yield rate(RNH_(3))of 1476.9±62.6μg h^(−1)cm^(−2)at−0.7 V(vs.reversible hydrogen electrode,RHE)and a faradaic efficiency(FE)of 89.0±3.8%at−0.5 V(vs.RHE)under ambient conditions.Further,when evaluated with a practical flow cell,Mn-O-C shows a high RNH_(3)of 3706.7±552.0μg h^(−1)cm^(−2)at a current density of 100 mA cm−2,2.5 times of that in the H cell.The in situ FT-IR and Raman spectroscopic studies combined with theoretical calculations indicate that the Mn-(O-C_(2))_(4)sites not only effectively inhibit the competitive hydrogen evolution reaction,but also greatly promote the adsorption and activation of nitrate(NO_(3)^(−)),thus boosting both the FE and selectivity of NH_(3)over Mn-(O-C_(2))_(4)sites. 展开更多
关键词 Atomically dispersed oxygen coordination Nitrate reduction reaction In situ spectroscopic studies hydrogen evolution reaction
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Efficient hydrogen peroxide production enabled by exploring layered metal telluride as two electron oxygen reduction reaction electrocatalyst
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作者 Yingming Wang Hongyuan Yang +6 位作者 Zhiwei Liu Kui Yin Zhaowu Wang Hui Huang Yang Liu Zhenhui Kang Ziliang Chen 《Journal of Energy Chemistry》 SCIE EI CSCD 2023年第12期247-255,I0007,共10页
It is of great interest to develop the novel transition metal-based electrocatalysts with high selectivity and activity for two electron oxygen reduction reaction(2e^(-) ORR).Herein,the nickel ditelluride(NiTe_(2)) wi... It is of great interest to develop the novel transition metal-based electrocatalysts with high selectivity and activity for two electron oxygen reduction reaction(2e^(-) ORR).Herein,the nickel ditelluride(NiTe_(2)) with layered structure was explored as the 2e^(-) ORR electrocatalyst,which not only showed the highest 2e^(-) selectivity more than 97%,but also delivered a slight activity decay after 5000 cycles in alkaline media.Moreover,when NiTe_(2) was assembled as the electrocatalyst in H-type electrolyzer,the on-site yield of H_(2)O_(2) could reach up to 672 mmol h^(-1)g^(-1) under 0.45 V vs.RHE.Further in situ Raman spectra,theoretical calculation and post microstructural analysis synergistically unveiled that such a good 2e^(-) ORR performance could be credited to the intrinsic layered crystal structure,the high compositional stability,as well as the electron modulation on the active site Ni atoms by neighboring Te atoms,leading to the exposure of active sites as well as the optimized adsorption free energy of Ni to –OOH.More inspiringly,such telluride electrocatalyst has also been demonstrated to exhibit high activity and selectivity towards 2e^(-) ORR in neutral media. 展开更多
关键词 Transition metal telluride oxygen reduction reaction Charge polarization Activity and selectivity hydrogen peroxide
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100 W-class green hydrogen production from ammonia at a dual-layer electrode containing a Pt-Ir catalyst for an alkaline electrolytic process
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作者 Donghyun Yoon Sunki Chung +2 位作者 Minjun Choi Eunhyeok Yang Jaeyoung Lee 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第6期352-360,I0009,共10页
Ammonia allows storage and transport of hydrogen over long distances and is an attractive potential hydrogen carrier.Electrochemical decomposition has recently been used for the conversion of ammonia to hydrogen and i... Ammonia allows storage and transport of hydrogen over long distances and is an attractive potential hydrogen carrier.Electrochemical decomposition has recently been used for the conversion of ammonia to hydrogen and is regarded as a future technology for production of CO_(2)-free pure hydrogen.Herein,a heterostructural Pt-Ir dual-layer electrode is developed and shown to achieve successful long-term operation in an ammonia electrolyzer with an anion exchange membrane(AEM).This electrolyzer consisted of eight membra ne electrode assemblies(MEAs)with a total geometric area of 200 cm~2 on the anode side,which resulted in a hydrogen production rate of 25 L h~(-1).We observed the degradation in MEA performance attributed to changes in the anode catalyst layer during hydrogen production via ammonia electrolysis.Furthermore,we demonstrated the relationship between the ammonia oxidation reaction(AOR)and the oxygen evolution reaction(OER). 展开更多
关键词 Ammonia oxidation Dual-layer catalyst Green hydrogen Electrolytic process oxygen evolution reaction
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Conducting Polymer-Based e-Refinery for Sustainable Hydrogen Peroxide Production
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作者 Zhixing Wu Penghui Ding +7 位作者 Viktor Gueskine Robert Boyd Eric Daniel G■owacki Magnus Odén Xaνier Crispin Magnus Berggren Emma M.Björk Mikhail Vagin 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2024年第2期334-342,共9页
Electrocatalysis enables the industrial transition to sustainable production of chemicals using abundant precursors and electricity from renewable sources.De-centralized production of hydrogen peroxide(H_(2)O_(2))from... Electrocatalysis enables the industrial transition to sustainable production of chemicals using abundant precursors and electricity from renewable sources.De-centralized production of hydrogen peroxide(H_(2)O_(2))from water and oxygen of air is highly desirable for daily life and industry.We report an effective electrochemical refinery(e-refinery)for H_(2)O_(2)by means of electrocatalysis-controlled comproportionation reaction(2_(H)O+o→2HO),feeding pure water and oxygen only.Mesoporous nickel(Ⅱ)oxide(NiO)was used as electrocatalyst for oxygen evolution reaction(OER),producing oxygen at the anode.Conducting polymer poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)(PEDOT:PSS)drove the oxygen reduction reaction(ORR),forming H_(2)O_(2)on the cathode.The reactions were evaluated in both half-cell and device configurations.The performance of the H_(2)O_(2)e-refinery,assembled on anion-exchange solid electrolyte and fed with pure water,was limited by the unbalanced ionic transport.Optimization of the operation conditions allowed a conversion efficiency of 80%. 展开更多
关键词 conducting polymer hydrogen peroxide nickel(Ⅱ)oxide oxygen evolution reaction oxygen reduction reaction
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Atomic-level coupled RuO_(2)/BaRuO_(3) heterostructure for efficient alkaline hydrogen evolution reaction
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作者 Yueying Yan Tian Meng +4 位作者 Yuting Chen Yang Yang Dewen Wang Zhicai Xing Xiurong Yang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第1期356-362,I0009,共8页
The slow water dissociation is the rate-determining step that slows down the reaction rate in alkaline hydrogen evolution reaction(HER).Optimizing the surface electronic structure of the catalyst to lower the energy b... The slow water dissociation is the rate-determining step that slows down the reaction rate in alkaline hydrogen evolution reaction(HER).Optimizing the surface electronic structure of the catalyst to lower the energy barrier of water dissociation and regulating the binding strength of adsorption intermediates are crucial strategy for boosting the catalytic performance of HER.In this study,RuO_(2)/BaRuO_(3)(RBRO)heterostructures with abundant oxygen vacancies and lattice distortion were in-situ constructed under a low temperature via the thermal decomposition of gel-precursor.The RBRO heterostructures obtained at 550℃ exhibited the highest HER activity in 1 M KOH,showing an ultra-low overpotential of 16 mV at 10 mA cm^(-2)and a Tafel slope of 33.37 m V dec^(-1).Additionally,the material demonstrated remarkable durability,with only 25 mV of degradation in overpotential after 200 h of stability testing at 10 mA cm^(-2).Density functional theory calculations revealed that the redistribution of charges at the heterojunction interface can optimize the binding energies of H*and OH*and effectively lower the energy barrier of water dissociation.This research offers novel perspectives on surpassing the water dissociation threshold of alkaline HER catalysts by means of a systematic design of heterogeneous interfaces. 展开更多
关键词 HETEROSTRUCTURE hydrogen evolution reaction Interfacial electron transfer oxygen vacancies
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Pd^(0)-O v-Ce^(3+) Interfacial Sites with Charge Redistribution for Enhanced Hydrogenation of Methyl Oleate to Methyl Stearate
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作者 Zhaohui Meng Ying Liao +6 位作者 Ling Liu Yaqian Li Hao Yan Xiang Feng Xiaobo Chen Yibin Liu Chaohe Yang 《Transactions of Tianjin University》 EI CAS 2024年第4期359-368,共10页
Improving the efficiency of metal/reducible metal oxide interfacial sites for hydrogenation reactions of unsaturated groups(e.g.,C=C and C=O)is a promising yet challenging endeavor.In our study,we developed a Pd/CeO_(... Improving the efficiency of metal/reducible metal oxide interfacial sites for hydrogenation reactions of unsaturated groups(e.g.,C=C and C=O)is a promising yet challenging endeavor.In our study,we developed a Pd/CeO_(2) catalyst by enhancing the oxygen vacancy(O V)concentration in CeO_(2) through high-temperature treatment.This process led to the formation of an interface structure ideal for supporting the hydrogenation of methyl oleate to methyl stearate.Specifi cally,metal Pd^(0) atoms bonded to the O V in defective CeO_(2) formed Pd^(0)-O v-Ce^(3+)interfacial sites,enabling strong electron transfer from CeO_(2) to Pd.The interfacial sites exhibit a synergistic adsorption eff ect on the reaction substrate.Pd^(0) sites promote the adsorption and activation of C=C bonds,while O V preferably adsorbs C=O bonds,mitigating competition with C=C bonds for Pd^(0) adsorption sites.This synergy ensures rapid C=C bond activation and accelerates the attack of active H*species on the semi-hydrogenated intermediate.As a result,our Pd/CeO_(2)-500 catalyst,enriched with Pd^(0)-O v-Ce^(3+)interfacial sites,dem-onstrated excellent hydrogenation activity at just 30℃.The catalyst achieved a Cis-C18:1 conversion rate of 99.8% and a methyl stearate formation rate of 5.7 mol/(h·g metal).This work revealed the interfacial sites for enhanced hydrogenation reactions and provided ideas for designing highly active hydrogenation catalysts. 展开更多
关键词 hydrogenATION Interfacial sites oxygen vacancy C=C bond
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Marrying luminescent metal nanoclusters to C_(3)N_(4) for efficient photocatalytic hydrogen peroxide production
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作者 Zhen Jiang Ziqi Li +4 位作者 Qiuxia He Songjie Han Yong Liu Haiguang Zhu Xun Yuan 《Materials Reports(Energy)》 EI 2024年第2期83-89,共7页
Photocatalytic oxygen(O_(2))reduction has been considered a promising method for hydrogen peroxide(H_(2)O_(2))production.However,the poor visible light harvesting and low-efficient separation and generation of charge ... Photocatalytic oxygen(O_(2))reduction has been considered a promising method for hydrogen peroxide(H_(2)O_(2))production.However,the poor visible light harvesting and low-efficient separation and generation of charge carriers of conventional photocatalysts strongly limited their photocatalytic H_(2)O_(2) generation performance.Herein,we design a highly efficient photocatalyst in this work by marrying luminescent gold-silver nanoclusters(AuAg NCs)to polyethyleneimine(PEI)modified C_(3)N_(4)(C3N4-PEI).The key design in this work is the utilization of highly luminescent AuAg NCs as photosensitizers to promote the generation and separation of charge carriers of C_(3)N_(4)-PEI,thereby ultimately producing abundant e−for O_(2) reduction under visible light illumination(λ≥400 nm).As a result,the as-designed photocatalyst(C3N4-PEI-AuAg NCs)exhibits excellent photocatalytic activity with an H_(2)O_(2) production capability of 82μM in pure water,which is 3.5 times higher than pristine C_(3)N_(4)(23μM).This interesting design provides a paradigm in developing other high-efficient photocatalysts for visible-light-driven H_(2)O_(2) production. 展开更多
关键词 Visible-light-driven oxygen reduction Metal nanoclusters Graphitic carbon nitride hydrogen peroxide production
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Solar Driven 15.7% Hydrogen Conversion by Harmony of Light Harvesting,Electron Transporting Bridge,and S-Defection in a Self-Assembled Microscale CuS/rGO/CP Photoanode
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作者 Sujeong Kim Boseok Seo +6 位作者 Hyerim Park Younghwan Im Jeong Yeon Do Byung Sub Kwak Namgyu Son Minkyu Kim Misook Kang 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2024年第3期190-201,共12页
CuS is an encouraging photoelectrode candidate that meets the essential requirements for efficient solar-to-hydrogen production,but it has not been thoroughly studied.A CuS light absorber layer is grown by the self-as... CuS is an encouraging photoelectrode candidate that meets the essential requirements for efficient solar-to-hydrogen production,but it has not been thoroughly studied.A CuS light absorber layer is grown by the self-assembly of copper and sulfur precursors on a carbon paper(CP)electrode.Simultaneously,rGO is introduced as a buffer layer to control the optical and electrical properties of the absorber.The well-ordered microstructural arrangement suppresses the recombination loss of electrons and holes owing to enhanced charge-carrier generation,separation,and transport.The potential reaching 10 mA cm^(-2)in 1.0 M KOH solution is significantly lowered to 0.87 V,and the photocurrent density at 1.23 V is 94.7 mA cm^(-2).The computational result reveals that the potential-determining step is sensitive to O^(*)stability;the lower stability of O^(*)in the thin layer of CuS/rGO decreases the free-energy gap between the initial and final states of the potential-determining step,resulting in a lowering of the onset potential.The faradaic efficiency for the photoelectrochemical oxygen evolution reaction in the optimized 2CuS/1rGO/CP photoanode is 98.60%,and the applied bias photon-to-current and the solar-to-hydrogen efficiencies are 11.2%and 15.7%,respectively,and its ultra-high performance is maintained for 250 h.These record-breaking achievement indices may be a trigger for establishing a green hydrogen economy. 展开更多
关键词 15.7%-solar to hydrogen density functional theory lower photopotential p-CuS/rGO/CP photoanode photoelectrochemical oxygen evolution
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Hydrogen sulfide reduces oxidative stress in Huntington's disease via Nrf2
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作者 Zige Jiang Dexiang Liu +7 位作者 Tingting Li Chengcheng Gai Danqing Xin Yijing Zhao Yan Song Yahong Cheng Tong Li Zhen Wang 《Neural Regeneration Research》 SCIE CAS 2025年第6期1776-1788,共13页
The pathophysiology of Huntington's disease involves high levels of the neurotoxin quinolinic acid. Quinolinic acid accumulation results in oxidative stress, which leads to neurotoxicity. However, the molecular an... The pathophysiology of Huntington's disease involves high levels of the neurotoxin quinolinic acid. Quinolinic acid accumulation results in oxidative stress, which leads to neurotoxicity. However, the molecular and cellular mechanisms by which quinolinic acid contributes to Huntington's disease pathology remain unknown. In this study, we established in vitro and in vivo models of Huntington's disease by administering quinolinic acid to the PC12 neuronal cell line and the striatum of mice, respectively. We observed a decrease in the levels of hydrogen sulfide in both PC12 cells and mouse serum, which was accompanied by down-regulation of cystathionine β-synthase, an enzyme responsible for hydrogen sulfide production. However, treatment with NaHS(a hydrogen sulfide donor) increased hydrogen sulfide levels in the neurons and in mouse serum, as well as cystathionine β-synthase expression in the neurons and the mouse striatum, while also improving oxidative imbalance and mitochondrial dysfunction in PC12 cells and the mouse striatum. These beneficial effects correlated with upregulation of nuclear factor erythroid 2-related factor 2 expression. Finally, treatment with the nuclear factor erythroid 2-related factor 2inhibitor ML385 reversed the beneficial impact of exogenous hydrogen sulfide on quinolinic acid-induced oxidative stress. Taken together, our findings show that hydrogen sulfide reduces oxidative stress in Huntington's disease by activating nuclear factor erythroid 2-related factor 2,suggesting that hydrogen sulfide is a novel neuroprotective drug candidate for treating patients with Huntington's disease. 展开更多
关键词 apoptosis CYSTATHIONINE-Β-SYNTHASE nuclear factor erythroid 2-related factor 2 Huntington's disease hydrogen sulfide MITOCHONDRION NEUROPLASTICITY oxidative stress quinolinic acid reactive oxygen species
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Oxygen and Hydrogen Isotopes of Waters in the Ordos Basin,China:Implications for Recharge of Groundwater in the North of Cretaceous Groundwater Basin 被引量:10
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作者 YANG Yuncheng SHEN Zhaoli +4 位作者 WENG Dongguang HOU Guangcai ZHAO Zhenhong WANG Dong PANG Zhonghe 《Acta Geologica Sinica(English Edition)》 SCIE CAS CSCD 2009年第1期103-113,共11页
Hundreds of precipitation samples collected from meteorological stations in the Ordos Basin from January 1988 to December 2005 were used to set up a local meteoric water line and to calculate weighted average isotopic... Hundreds of precipitation samples collected from meteorological stations in the Ordos Basin from January 1988 to December 2005 were used to set up a local meteoric water line and to calculate weighted average isotopic compositions of modern precipitation. Oxygen and hydrogen isotopes, with averages of-7.8‰ and -53.0‰ for δ^18O and δD, respectively, are depleted in winter and rich in spring, and gradually decrease in summer and fall, illustrating that the seasonal effect is considerable. They also show that the isotopic difference between south portion and north portion of the Ordos Basin are not obvious, and the isotope in the middle portion is normally depleted. The isotope compositions of 32 samples collected from shallow groundwater (less than a depth of 150 m) in desert plateau range from -10.6‰ to -6.0‰ with an average of-8.4‰ for δ^18O and from -85‰ to -46‰ with an average of-63‰ for δD. Most of them are identical with modern precipitation. The isotope compositions of 22 middle and deep groundwaters (greater than a depth of 275 m) fall in ranges from -11.6‰ to -8.8‰ with an average of -10.2‰ for δ^18O and from -89‰ to -63‰ with an average of -76‰ for δD. The average values are significantly less than those of modern precipitation, illustrating that the middle and deep groundwaters were recharged at comparatively lower air temperatures. Primary analysis of ^14C shows that the recharge of the middle and deep groundwaters started at late Pleistocene. The isotopes of 13 lake water samples collected from eight lakes define a local evaporation trend, with a relatively flat slope of 3.77, and show that the lake waters were mainly fed by modern precipitation and shallow groundwater. 展开更多
关键词 GROUNDWATER lake water oxygen and hydrogen isotopes precipitation Ordos Basin
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Estimating distribution of water uptake with depth of winter wheat by hydrogen and oxygen stable isotopes under different irrigation depths 被引量:10
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作者 GUO Fei MA Juan-juan +3 位作者 ZHENG Li-jian SUN Xi-huan GUO Xiang-hong ZHANG Xue-lan 《Journal of Integrative Agriculture》 SCIE CAS CSCD 2016年第4期891-906,共16页
Crop root system plays an important role in the water cycle of the soil-plant-atmosphere continuum. In this study, com- bined isotope techniques, root length density and root cell activity analysis were used to invest... Crop root system plays an important role in the water cycle of the soil-plant-atmosphere continuum. In this study, com- bined isotope techniques, root length density and root cell activity analysis were used to investigate the root water uptake mechanisms of winter wheat (Triticum aesfivum L.) under different irrigation depths in the North China Plain. Both direct inference approach and multisource linear mixing model were applied to estimate the distribution of water uptake with depth in six growing stages. Results showed that winter wheat under land surface irrigation treatment (Ts) mainly absorbed water from 10-20 cm soil layers in the wintering and green stages (66.9 and 72.0%, respectively); 0-20 cm (57.0%) in the jointing stage; 0-40 (15.3%) and 80-180 cm (58.1%) in the heading stage; 60-80 (13.2%) and 180-220 cm (35.5%) in the filling stage; and 0-40 (46.8%) and 80-100 cm (31.0%) in the ripening stage. Winter wheat under whole soil layers irrigation treatment (Tw) absorbed more water from deep soil layer than Ts in heading, filling and ripening stages. Moreover, root cell activity and root length density of winter wheat under TW were significantly greater than that of Ts in the three stages. We concluded that distribution of water uptake with depth was affected by the availability of water sources, the root length density and root cell activity. Implementation of the whole soil layers irrigation method can affect root system distribution and thereby increase water use from deeper soil and enhance water use efficiency. 展开更多
关键词 hydrogen and oxygen stable isotopes multisource linear mixing model winter wheat distribution of wateruptake with depth
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