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Enhanced photocatalytic hydrogen production of S-scheme TiO_(2)/g-C_(3)N_(4)heterojunction loaded with single-atom Ni 被引量:2
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作者 Songyu Yang Kailin Wang +1 位作者 Qiao Chen Yan Wu 《Journal of Materials Science & Technology》 SCIE EI CAS CSCD 2024年第8期104-114,共11页
S-scheme heterostructure photocatalysts can achieve highly efficient solar energy utilization.Here,singleatom Ni species were deposited onto TiO_(2)/g-C_(3)N_(4)(TCN)composite photocatalyst with an S-scheme het-erojun... S-scheme heterostructure photocatalysts can achieve highly efficient solar energy utilization.Here,singleatom Ni species were deposited onto TiO_(2)/g-C_(3)N_(4)(TCN)composite photocatalyst with an S-scheme het-erojunction for highly efficient photocatalytic water splitting to produce hydrogen.Under solar irradiation,it realized the hydrogen production activity of 134μmol g^(-1)h^(-1),about 5 times higher than the TCN without atomic Ni.Insitu Kelvin probe force microscopy characterization and the density functional cal-culation certify that by forming the S-scheme heterojunction,the photo-excited electrons from the TiO_(2)combine with the photogenerated holes at the coupled g-C_(3)N_(4)driven by a built-in electric field.More importantly,the single-atom Ni species stabilized the photogenerated electrons from the g-C_(3)N_(4)could effectively enhance the charge separation between the holes on the valence band of TiO_(2)and electrons at the conduction band of g-C_(3)N_(4).Meanwhile,the Ni atoms act as the surface catalytic centers for the water reduction reaction,which greatly improves the reactivity of the photocatalyst.The present work provides a new approach for developing noble metal-free heterojunctions for high-efficiency photocatalysis. 展开更多
关键词 S-scheme Single-atom catalysis TiO_(2)/g-C_(3)N_(4) hydrogen production Built-in electric field
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Classification and technical target of water electrolysis for hydrogen production
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作者 Kahyun Ham Sooan Bae Jaeyoung Lee 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第8期554-576,I0012,共24页
Continuous efforts are underway to reduce carbon emissions worldwide in response to global climate change.Water electrolysis technology,in conjunction with renewable energy,is considered the most feasible hydrogen pro... Continuous efforts are underway to reduce carbon emissions worldwide in response to global climate change.Water electrolysis technology,in conjunction with renewable energy,is considered the most feasible hydrogen production technology based on the viable possibility of large-scale hydrogen production and the zero-carbon-emission nature of the process.However,for hydrogen produced via water electrolysis systems to be utilized in various fields in practice,the unit cost of hydrogen production must be reduced to$1/kg H_(2).To achieve this unit cost,technical targets for water electrolysis have been suggested regarding components in the system.In this paper,the types of water electrolysis systems and the limitations of water electrolysis system components are explained.We suggest guideline with recent trend for achieving this technical target and insights for the potential utilization of water electrolysis technology. 展开更多
关键词 Water electrolysis hydrogen production Technical target ELECTROCHEMISTRY
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Asymmetric orbital hybridization in Zn-doped antiperovskite Cu_(1-x)Zn_(x)NMn_(3)enables highly efficient electrocatalytic hydrogen production
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作者 Yuxiang Yan Yuxin Cao +9 位作者 Zhichao Wang Ka Wang Hengdong Ren Shaoqi Zhang Yi Wang Jian Chen Yong Zhou Lizhe Liu Jun Dai Xinglong Wu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第2期304-312,I0008,共10页
Rational design of efficient and robust earth-abundant alkaline hydrogen evolution reaction(HER)catalysts is a key factor for developing energy conversion technologies.Currently,antiperovskite nitride CuNMn_(3)has gar... Rational design of efficient and robust earth-abundant alkaline hydrogen evolution reaction(HER)catalysts is a key factor for developing energy conversion technologies.Currently,antiperovskite nitride CuNMn_(3)has garnered significant interest due to its remarkable properties such as negative/zero thermal expansion and magnetocaloric effects.However,when utilized as hydrogen evolution catalysts,it encounters large challenge resulting from excessively strong/weak interactions with adsorbed H on Mn/Cu active sites,which leads to low HER activity.In this study,we introduce an asymmetric orbital hybridization strategy in Zn-doped Cu_(1-x)Zn_(x)NMn_(3)by leveraging the localization of Zn electronic states to reconfigure the electronic structures of Cu and Mn,thereby reducing the energy barrier for water dissociation and optimizing Cu and Mn active sites for hydrogen adsorption and H_(2)production.Electrochemical evaluations reveal that Cu_(0.85)Zn_(0.15)NMn_(3)with x=0.15 demonstrates exceptional electrocatalytic activity in alkaline electrolytes.A low overpotential of 52 mV at 10 mA cm^(-2)and outstanding stability over a 150-h test period are achieved,surpassing commercial Pt/C.This research offers a novel strategy for enhancing HER performance by modulating asymmetric hybridization of electron orbitals between multiple metal atoms within a material structure. 展开更多
关键词 Cu_(1-x)ZnxNMn_(3) Asymmetric orbital hybridization hydrogen adsorption hydrogen production
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Amorphous Iridium Oxide-Integrated Anode Electrodes with Ultrahigh Material Utilization for Hydrogen Production at Industrial Current Densities
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作者 Lei Ding Kui Li +10 位作者 Weitian Wang Zhiqiang Xie Shule Yu Haoran Yu David ACullen Alex Keane Kathy Ayers Christopher BCapuano Fangyuan Liu Pu-Xian Gao Feng-Yuan Zhang 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第10期225-239,共15页
Herein,ionomer-free amorphous iridium oxide(IrO_(x))thin electrodes are first developed as highly active anodes for proton exchange membrane electrolyzer cells(PEMECs)via low-cost,environmentally friendly,and easily s... Herein,ionomer-free amorphous iridium oxide(IrO_(x))thin electrodes are first developed as highly active anodes for proton exchange membrane electrolyzer cells(PEMECs)via low-cost,environmentally friendly,and easily scalable electrodeposition at room temperature.Combined with a Nafion 117 membrane,the IrO_(x)-integrated electrode with an ultralow loading of 0.075 mg cm^(-2)delivers a high cell efficiency of about 90%,achieving more than 96%catalyst savings and 42-fold higher catalyst utilization compared to commercial catalyst-coated membrane(2 mg cm^(-2)).Additionally,the IrO_(x)electrode demonstrates superior performance,higher catalyst utilization and significantly simplified fabrication with easy scalability compared with the most previously reported anodes.Notably,the remarkable performance could be mainly due to the amorphous phase property,sufficient Ir^(3+)content,and rich surface hydroxide groups in catalysts.Overall,due to the high activity,high cell efficiency,an economical,greatly simplified and easily scalable fabrication process,and ultrahigh material utilization,the IrO_(x)electrode shows great potential to be applied in industry and accelerates the commercialization of PEMECs and renewable energy evolution. 展开更多
关键词 Ionomer-free Amorphous IrOx electrodes Ultrahigh material utilization Scalable electrodeposition hydrogen production
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Decoupled water electrolysis:Flexible strategy for pure hydrogen production with small voltage inputs
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作者 Kexin Zhou Jiahui Huang +3 位作者 Daili Xiang Aijiao Deng Jialei Du Hong Liu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第7期340-356,共17页
Hydrogen gas is widely regarded as an ideal green energy carrier and a potential alternative to fossil fuels for coping with the aggravating energy crisis and environmental pollution.Currently,the vast majority of the... Hydrogen gas is widely regarded as an ideal green energy carrier and a potential alternative to fossil fuels for coping with the aggravating energy crisis and environmental pollution.Currently,the vast majority of the world's hydrogen is produced by reforming fossil fuels;however,this hydrogen-making technology is not sustainable or environmentally friendly because ofits high energy consumption and large carbon emissions.Renewables-driven water splitting(2H_(2)0-2H_(2)+0_(2))becomes an extensively studied scheme for sustain-able hydrogen production.Conventional water electrolysis requires an input voltage higher than 1.23 V and forms a gas mixture of H_(2)/O_(2),which results in high electricity consumption,potential safety hazards,and harmful reactive oxygen species.By virtue of the auxiliary redox mediators(RMs)as the robust H^(+)/e^(-)reservoir,decoupled electrolysis splits water at a much lower potential and evolves O_(2)(H_(2)O+RMS_(ox)-O_(2)+H-RMS_(red))and H_(2)(H-RMS_(red)-H_(2)+RMS_(ox))at separate times,rates,and spaces,thus pro-ducing the puretarget hydrogen gas safely.Decoupled electrolysis has accelerated the development ofwater electrolysis technology for H_(2) production.However,itis still lack of a comprehensive and in-depth review in this field based on different types of RMs.This review highlights the basic principles and critical progress of this emerging water electrolysis mode over the past decade.Several representative examples are then dis-played in detail according to the differences in the RMs.The rational choice and design of RMs have also been emphasized.Subsequently,novel applications of decoupled water splitting are briefly discussed,including the manufacture of valuable chemicals,Cl_(2) production,pollutant degradation,and other half-reactions in artificial photosynthesis.Finally,thekey characteristics and disadvantages of each type of mediator are sum-marized in depth.In addition,we present an outlook for future directions in decoupled water splitting.Thus,the flexibility in the design of mediators provides huge space for improving this electrochemical technology.@2024 Science Press and Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by ELSEVIER B.V.and Science Press.All rights reserved. 展开更多
关键词 hydrogen production Conventional water splitting Decoupled water splitting Redox mediators Biomimetics
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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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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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Ethanol steam reforming over Ni/ZSM-5 nanosheet for hydrogen production
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作者 Porapak Suriya Shanshan Xu +8 位作者 Shengzhe Ding Sarayute Chansai Yilai Jiao Joseph Hurd Daniel Lee Yuxin Zhang Christopher Hardacre Prasert Reubroycharoen Xiaolei Fan 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第3期247-256,共10页
Compared to reforming reactions using hydrocarbons,ethanol steam reforming(ESR)is a sustainable alternative for hydrogen(H_(2))production since ethanol can be produced sustainably using biomass.This work explores the ... Compared to reforming reactions using hydrocarbons,ethanol steam reforming(ESR)is a sustainable alternative for hydrogen(H_(2))production since ethanol can be produced sustainably using biomass.This work explores the catalyst design strategies for preparing the Ni supported on ZSM-5 zeolite catalysts to promote ESR.Specifically,two-dimensional ZSM-5 nanosheet and conventional ZSM-5 crystal were used as the catalyst carriers and two synthesis strategies,i.e.,in situ encapsulation and wet impregnation method,were employed to prepare the catalysts.Based on the comparative characterization of the catalysts and comparative catalytic assessments,it was found that the combination of the in situ encapsulation synthesis and the ZSM-5 nanosheet carrier was the effective strategy to develop catalysts for promoting H_(2) production via ESR due to the improved mass transfer(through the 2-D structure of ZSM-5 nanosheet)and formation of confined small Ni nanoparticles(resulted via the in situ encapsulation synthesis).In addition,the resulting ZSM-5 nanosheet supported Ni catalyst also showed high Ni dispersion and high accessibility to Ni sites by the reactants,being able to improve the activity and stability of catalysts and suppress metal sintering and coking during ESR at high reaction temperatures.Thus,the Ni supported on ZSM-5 nanosheet catalyst prepared by encapsulation showed the stable performance with~88% ethanol conversion and~65% H_(2) yield achieved during a 48-h longevity test at 550-C. 展开更多
关键词 ZSM-5 nanosheet In situ encapsulation Ni catalyst Ethanol steam reforming hydrogen production
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Biological Hydrogen Production:A Comprehensive Review for Converting Wastes into Wealth
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作者 Tongming Li Fei Gao Yigeng Huangfu 《Chinese Journal of Electrical Engineering》 EI CSCD 2024年第3期110-134,共25页
Energy shortages have hindered global economic development.By utilizing waste as a substrate for microbial fermentation,hydrogen production can transform waste into a valuable resource,significantly reducing the cost ... Energy shortages have hindered global economic development.By utilizing waste as a substrate for microbial fermentation,hydrogen production can transform waste into a valuable resource,significantly reducing the cost of hydrogen production and addressing a significant hurdle in achieving large-scale production of microbial hydrogen.This approach has significant potential for future hydrogen-production applications.Two-stage indirect photohydrolysis has recently emerged as a promising and efficient method for hydrogen production using cyanobacteria and green algae.However,this method cannot be directly applied to organic wastewater for hydrogen production.In contrast,dark fermentation by bacteria,particularly ethanol-type fermentation,is highly efficient for producing hydrogen.Therefore,the combination of the indirect photohydrolysis of algae and dark fermentation by bacteria is expected to significantly enhance the hydrogen-production capacity of organic wastewater,laying the groundwork for future large-scale microbial hydrogen production.This study reviews the main types and technical principles of microbial hydrogen production from waste,available waste types,research progress in the microbial hydrogen-production process,strategies to improve the hydrogen-production rate,and challenges faced during industrialization.Future research directions for microbial-waste hydrogen production are also proposed.The aim of this study is to provide a valuable reference for large-scale biological hydrogen-production research. 展开更多
关键词 Biological hydrogen production dark fermentation waste utilization INDUSTRIALIZATION green energy
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Pt nanoclusters modified porous g-C_(3)N_(4)nanosheets to significantly enhance hydrogen production by photocatalytic water reforming of methanol
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作者 Yi-Fei Liang Jin-Rong Lu +2 位作者 Shang-Kun Tian Wen-Quan Cui Li Liu 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第2期40-50,共11页
For the use of green hydrogen energy,it is crucial to have efficient photocatalytic activity for hydrogen generation by water reforming of methanol under mild conditions.Much attention has been paid to gC_(3)N_(4)as a... For the use of green hydrogen energy,it is crucial to have efficient photocatalytic activity for hydrogen generation by water reforming of methanol under mild conditions.Much attention has been paid to gC_(3)N_(4)as a promising photocatalyst for the generation of hydrogen.To improve the separation of photogenerated charge,porous nanosheet g-C_(3)N_(4)was modified with Pt nanoclusters(Pt/g-C_(3)N_(4))through impregnation and following photo-induced reduction.This catalyst showed excellent photocatalytic activity of water reforming of methanol fo r hydrogen production with a 17.12 mmol·g^(-1)·h^(-1)rate at room temperature,which was 311 times higher than that of the unmodified g-C_(3)N_(4).The strong interactions of Pt-N in Pt/g-C_(3)N_(4)constructed effective electron transfer channels to promote the separation of photogenerated electrons and holes effectively.In addition,in-situ infrared spectroscopy was used to investigate the intermediates of the hydrogen production reaction,which proved that methanol and water eventually turn into H_(2)and CO_(2)via formaldehyde and formate.This study provides insights for understanding the photocatalytic hydrogen production in the water reforming of methanol. 展开更多
关键词 Water reforming of methanol Photocatalysis g-C_(3)N_(4) Pt nanoclusters hydrogen production
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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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Progress in manipulating spin polarization for solar hydrogen production
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作者 Qian Yang Xin Tong Zhiming Wang 《Materials Reports(Energy)》 EI 2024年第1期43-57,共15页
Photocatalytic and photoelectrochemical water splitting using semiconductor materials are effective approaches for converting solar energy into hydrogen fuel.In the past few years,a series of photocatalysts/photoelect... Photocatalytic and photoelectrochemical water splitting using semiconductor materials are effective approaches for converting solar energy into hydrogen fuel.In the past few years,a series of photocatalysts/photoelectrocatalysts have been developed and optimized to achieve efficient solar hydrogen production.Among various optimization strategies,the regulation of spin polarization can tailor the intrinsic optoelectronic properties for retarding charge recombination and enhancing surface reactions,thus improving the solar-to-hydrogen(STH)efficiency.This review presents recent advances in the regulation of spin polarization to enhance spin polarized-dependent solar hydrogen evolution activity.Specifically,spin polarization manipulation strategies of several typical photocatalysts/photoelectrocatalysts(e.g.,metallic oxides,metallic sulfides,non-metallic semiconductors,ferroelectric materials,and chiral molecules)are described.In the end,the critical challenges and perspectives of spin polarization regulation towards future solar energy conversion are briefly provided. 展开更多
关键词 Spin polarization Solar energy conversion Photocatalytic hydrogen production Photoelectrochemical water splitting
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Generation of input spectrum for electrolysis stack degradation test applied to wind power PEM hydrogen production
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作者 Yanhui Xu Guanlin Li +1 位作者 Yuyuan Gui Zhengmao Li 《Global Energy Interconnection》 EI CSCD 2024年第4期462-474,共13页
Hydrogen production by proton exchange membrane electrolysis has good fluctuation adaptability,making it suitable for hydrogen production by electrolysis in fluctuating power sources such as wind power.However,current... Hydrogen production by proton exchange membrane electrolysis has good fluctuation adaptability,making it suitable for hydrogen production by electrolysis in fluctuating power sources such as wind power.However,current research on the durability of proton exchange membrane electrolyzers is insufficient.Studying the typical operating conditions of wind power electrolysis for hydrogen production can provide boundary conditions for performance and degradation tests of electrolysis stacks.In this study,the operating condition spectrum of an electrolysis stack degradation test cycle was proposed.Based on the rate of change of the wind farm output power and the time-averaged peak-valley difference,a fluctuation output power sample set was formed.The characteristic quantities that played an important role in the degradation of the electrolysis stack were selected.Dimensionality reduction of the operating data was performed using principal component analysis.Clustering analysis of the data segments was completed using an improved Gaussian mixture clustering algorithm.Taking the annual output power data of wind farms in Northwest China with a sampling rate of 1 min as an example,the cyclic operating condition spectrum of the proton-exchange membrane electrolysis stack degradation test was constructed.After preliminary simulation analysis,the typical operating condition proposed in this paper effectively reflects the impact of the original curve on the performance degradation of the electrolysis stack.This study provides a method for evaluating the degradation characteristics and system efficiency of an electrolysis stack due to fluctuations in renewable energy. 展开更多
关键词 hydrogen production by electrolysis of water Wind power Proton exchange membrane electrolyzer Gaussian mixture model Cyclic operating condition
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High-rate electrochemical H_(2)O_(2) production over multimetallic atom catalysts under acidic–neutral conditions
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作者 Yueyu Tong Jiaxin Liu +5 位作者 Bing-Jian Su Jenh-Yih Juang Feng Hou Lichang Yin Shi Xue Dou Ji Liang 《Carbon Energy》 SCIE EI CAS CSCD 2024年第1期44-62,共19页
Hydrogen peroxide(H_(2)O_(2))production by the electrochemical 2-electron oxygen reduction reaction(2e−ORR)is a promising alternative to the energy-intensive anthraquinone process,and single-atom electrocatalysts show... Hydrogen peroxide(H_(2)O_(2))production by the electrochemical 2-electron oxygen reduction reaction(2e−ORR)is a promising alternative to the energy-intensive anthraquinone process,and single-atom electrocatalysts show the unique capability of high selectivity toward 2e−ORR against the 4e−one.The extremely low surface density of the single-atom sites and the inflexibility in manipulating their geometric/electronic configurations,however,compromise the H_(2)O_(2) yield and impede further performance enhancement.Herein,we construct a family of multiatom catalysts(MACs),on which two or three single atoms are closely coordinated to form high-density active sites that are versatile in their atomic configurations for optimal adsorption of essential*OOH species.Among them,the Cox–Ni MAC presents excellent electrocatalytic performance for 2e−ORR,in terms of its exceptionally high H_(2)O_(2) yield in acidic electrolytes(28.96 mol L^(−1) gcat.^(−1) h^(−1))and high selectivity under acidic to neutral conditions in a wide potential region(>80%,0–0.7 V).Operando X-ray absorption and density functional theory analyses jointly unveil its unique trimetallic Co2NiN8 configuration,which efficiently induces an appropriate Ni–d orbital filling and modulates the*OOH adsorption,together boosting the electrocatalytic 2e−ORR capability.This work thus provides a new MAC strategy for tuning the geometric/electronic structure of active sites for 2e−ORR and other potential electrochemical processes. 展开更多
关键词 hydrogen peroxide production multiatom catalysts operando X-ray adsorption spectrum reaction mechanism tendency structure-property relation
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Long-range electron synergy over Pt_(1)-Co_(1)/CN bimetallic single-atom catalyst in enhancing charge separation for photocatalytic hydrogen production 被引量:2
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作者 Man Yang Jing Mei +3 位作者 Yujing Ren Jie Cui Shuhua Liang Shaodong Sun 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第6期502-509,I0011,共9页
The development of novel single-atom catalysts with optimal electron configuration and economical noble-metal cocatalyst for efficient photocatalytic hydrogen production is of great importance,but still challenging.He... The development of novel single-atom catalysts with optimal electron configuration and economical noble-metal cocatalyst for efficient photocatalytic hydrogen production is of great importance,but still challenging.Herein,we fabricate Pt and Co single-atom sites successively on polymeric carbon nitride(CN).In this Pt_(1)-Co_(1)/CN bimetallic single-atom catalyst,the noble-metal active sites are maximized,and the single-atomic Co_(1)N_4sites are tuned to Co_(1)N_3sites by photogenerated electrons arising from the introduced single-atomic Pt_(1)N_4sites.Mechanism studies and density functional theory(DFT)calculations reveal that the 3d orbitals of Co_(1)N_3single sites are filled with unpaired d-electrons,which lead to the improved visible-light response,carrier separation and charge migration for CN photocatalysts.Thereafter,the protons adsorption and activation are promoted.Taking this advantage of long-range electron synergy in bimetallic single atomic sites,the photocatalytic hydrogen evolution activity over Pt_(1)-Co_(1)/CN achieves 915.8 mmol g^(-1)Pt h^(-1),which is 19.8 times higher than Co_(1)/CN and 3.5 times higher to Pt_(1)/CN.While this electron-synergistic effect is not so efficient for Pt nanoclusters.These results demonstrate the synergistic effect at electron-level and provide electron-level guidance for the design of efficient photocatalysts. 展开更多
关键词 Bimetallic single-atom catalyst Long-range electron synergy Charge separation/transfer Carbon nitride hydrogen production
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Preparation of TiO_(2) Supported Mxene Catalyst for High Efficiency Hydrogen Production 被引量:1
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作者 HU Mei XIN Jin +2 位作者 LIU Zhenyu ZENG Hui WANG Yanze 《Journal of Wuhan University of Technology(Materials Science)》 SCIE EI CAS CSCD 2023年第2期286-291,共6页
We studied a method to prepare a novel titanium dioxide(TiO_(2))composite photocatalyst,starting from improving the separation efficiency of photogenerated electrons and holes.Regular TiO_(2)microspheres were prepared... We studied a method to prepare a novel titanium dioxide(TiO_(2))composite photocatalyst,starting from improving the separation efficiency of photogenerated electrons and holes.Regular TiO_(2)microspheres were prepared by sol-gel method and loaded onto Ti3C2Tx(Mxene).The high electrical conductivity of Mxene was utilized to transfer photogenerated electrons quickly and effectively prevent their recombination.By adjusting the addition amount of Mxene,the hydrogen production efficiency of the sample was greatly improved,and the maximum efficiency reached 135.2μmol·g^(-1)·h^(-1),which was twice that of pure TiO_(2).The nanocomposites were characterized by XRD,PL,TEM and SEM analysis and electrochemical methods,and the test proved that the improvement of hydrogen production efficiency was caused by the improvement of the separation efficiency of photogenerated electrons and holes.This work demonstrates the application of Mxene as a catalyst to improve efficiency and broadens the application prospects of Mxene. 展开更多
关键词 TiO_(2) Mxene hydrogen production PHOTOCATALYSIS
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Ultralow-voltage hydrogen production and simultaneous Rhodamine B beneficiation in neutral wastewater 被引量:1
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作者 Xiang Peng Song Xie +8 位作者 Shijian Xiong Rong Li Peng Wang Xuming Zhang Zhitian Liu Liangsheng Hu Biao Gao Peter Kelly Paul K.Chu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第6期574-582,I0013,共10页
Electrocatalytic water splitting for hydrogen production is hampered by the sluggish oxygen evolution reaction(OER)and large power consumption and replacing the OER with thermodynamically favourable reactions can impr... Electrocatalytic water splitting for hydrogen production is hampered by the sluggish oxygen evolution reaction(OER)and large power consumption and replacing the OER with thermodynamically favourable reactions can improve the energy conversion efficiency.Since iron corrodes easily and even self-corrodes to form magnetic iron oxide species and generate corrosion currents,a novel strategy to integrate the hydrogen evolution reaction(HER)with waste Fe upgrading reaction(FUR)is proposed and demonstrated for energy-efficient hydrogen production in neutral media.The heterostructured MoSe_(2)/MoO_(2) grown on carbon cloth(MSM/CC)shows superior HER performance to that of commercial Pt/C at high current densities.By replacing conventional OER with FUR,the potential required to afford the anodic current density of 10 m A cm^(-2)decreases by 95%.The HER/FUR overall reaction shows an ultralow voltage of 0.68 V for 10 m A cm^(-2)with a power equivalent of 2.69 k Wh per m^(3)H_(2).Additionally,the Fe species formed at the anode extract the Rhodamine B(Rh B)pollutant by flocculation and also produce nanosized magnetic powder and beneficiated Rh B for value-adding applications.This work demonstrates both energy-saving hydrogen production and pollutant recycling without carbon emission by a single system and reveals a new direction to integrate hydrogen production with environmental recovery to achieve carbon neutrality. 展开更多
关键词 Energy-saving hydrogen production hydrogen evolution reaction Neutral water splitting MoSe_(2)/MoO_(2)heterostructure Environmental recovery
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Low-content Pt-triggered the optimized d-band center of Rh metallene for energy-saving hydrogen production coupled with hydrazine degradation 被引量:1
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作者 Qiqi Mao Wenxin Wang +6 位作者 Kai Deng Hongjie Yu Ziqiang Wang You Xu Xiaonian Li Liang Wang Hongjing Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第10期58-66,I0004,共10页
Utilizing the hydrazine-assisted water electrolysis for energy-efficient hydrogen production shows a promising application, which relies on the development and design of efficient bifunctional electrocatalysts. Herein... Utilizing the hydrazine-assisted water electrolysis for energy-efficient hydrogen production shows a promising application, which relies on the development and design of efficient bifunctional electrocatalysts. Herein, we reported a low-content Pt-doped Rh metallene(Pt-Rhene) for hydrazine-assisted water electrolysis towards energy-saving hydrogen(H_(2)) production, where the ultrathin metallene is constructed to provide enough favorable active sites for catalysis and improve atom utilization.Additionally, the synergistic effect between Rh and Pt can optimize the electronic structure of Rh for improving the intrinsic activity. Therefore, the required overpotential of Pt-Rhene is only 37 mV to reach a current density of-10 mA cm^(-2) in the hydrogen evolution reaction(HER), and the Pt-Rhene exhibits a required overpotential of only 11 mV to reach a current density of 10 mA cm^(-2) in the hydrazine oxidation reaction(HzOR). With the constructed HER-HzOR two-electrode system, the Pt-Rhene electrodes exhibit an extremely low voltage(0.06/0.19/0.28 V) to achieve current densities of 10/50/100 mA cm^(-2) for energy-saving H_(2) production, which greatly reduces the electrolysis energy consumption. Moreover,DFT calculations further demonstrate that the introduction of Pt modulates the electronic structure of Rh and optimizes the d-band center, thus enhancing the adsorption and desorption of reactant/intermediates in the electrocatalytic reaction. 展开更多
关键词 Pt-Rhene Synergistic effect hydrogen evolution reaction Hydrazine oxidation reaction Energy-saving H_(2)production
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Air-condition process for scalable fabrication of CdS/ZnS 1D/2D heterojunctions toward efficient and stable photocatalytic hydrogen production
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作者 Dongdong Zhang Jie Teng +7 位作者 Hongli Yang Zhi Fang Kai Song Lin Wang Huilin Hou Xianlu Lu Chris RBowen Weiyou Yang 《Carbon Energy》 SCIE CSCD 2023年第7期1-14,共14页
We report the scalable fabrication of CdS/ZnS 1D/2D heterojunctions under ambient air conditions(i.e.,room temperature and atmospheric pressure)in which ZnS nanoparticles are anchored on the surface of CdS nanosheets.... We report the scalable fabrication of CdS/ZnS 1D/2D heterojunctions under ambient air conditions(i.e.,room temperature and atmospheric pressure)in which ZnS nanoparticles are anchored on the surface of CdS nanosheets.The as-formed heterojunctions exhibit a significantly enhanced photocatalytic H_(2) evolution rate of 14.02 mmol h^(-1) g^(-1) when irradiated with visible light,which is~10 and 85 times higher than those of pristine CdS nanosheets and CdS nanoparticles,respectively,and superior to most of the CdS-based photocatalysts reported to date.Furthermore,they provide robust photocatalytic performance with demonstratable stability over 58 h,indicating their potential for practical applications.The formation of 1D/2D heterojunctions not only provides improved exposed active sites that respond to illumination but also provides a rapid pathway to generate photogenerated carriers for efficient separation and transfer through the matrix of single-crystalline CdS nanosheets.In addition,first-principles simulations demonstrate that the existence of rich Zn vacancies increases the energy level of the ZnS valence band maximum to construct type-II and Z-scheme mixed heterojunctions,which plays a critical role in suppressing the recombination of carriers with limited photocorrosion of CdS to enhance photocatalytic behavior. 展开更多
关键词 air condition CDS HETEROJUNCTIONS photocatalytic hydrogen production ZNS
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Hydrogen production at intermediate temperatures with proton conducting ceramic cells:Electrocatalytic activity,durability and energy efficiency
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作者 Haoyu Zheng Feng Han +1 位作者 Noriko Sata Rémi Costa 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第11期437-446,I0010,共11页
Proton conducting ceramic cells(PCCs)are an attractive emerging technology operating in the intermediate temperature range of 500 to 700℃.In this work,we evaluate the production of hydrogen at intermediate temperatur... Proton conducting ceramic cells(PCCs)are an attractive emerging technology operating in the intermediate temperature range of 500 to 700℃.In this work,we evaluate the production of hydrogen at intermediate temperatures by proton conducting ceramic cell electrolysis(PCCEL).We demonstrate a highperformance steam electrolysis owing to a composite positrode based on BaGd_(0.8)La_(0.2)Co_(2)O_(6-δ)(BGLC1082)and BaZr0.5Ce0.4Y0.1O3-δ(BZCY541).The high reliability of PCCEL is demonstrated for 1680 h at a current density as high as-0.8 A cm^(-2)close to the thermoneutral cell voltage at 600℃.The electrolysis cell showed a specific energy consumption ranging from 54 to 66 kW h kg^(-1)that is comparable to state-of-the-art low temperature electrolysis technologies,while showing hydrogen production rates systematically higher than commercial solid oxide ceramic cells(SOCs).Compared to SOCs,the results verified the higher performances of PCCs at the relevant operating temperatures,due to the lower activation energy for proton transfer comparing with oxygen ion conduction.However,because of the p-type electronic conduction in protonic ceramics,the energy conversion rate of PCCs is relatively lower in steam electrolysis.The faradaic efficiency of the PCC in electrolysis mode can be increased at lower operating temperatures and in endothermic conditions,making PCCEL a technology of choice to valorize high temperature waste heat from industrial processes into hydrogen.To increase the faradaic efficiency by optimizing the materials,the cell design,or the operating strategy is a key challenge to address for future developments of PCCEL in order to achieve even more superior techno-economic merits. 展开更多
关键词 Steam electrolysis hydrogen production Proton conducting ceramics Intermediate temperature Energy efficiency
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