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Oxygen reduction electrocatalysis:From conventional to single-atomic platinum-based catalysts for proton exchange membrane fuel cells
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作者 Cheng YUAN Shiming ZHANG Jiujun ZHANG 《Frontiers in Energy》 SCIE EI CSCD 2024年第2期206-222,共17页
Platinum(Pt)-based materials are still the most efficient and practical catalysts to drive the sluggish kinetics of cathodic oxygen reduction reaction(ORR)in proton exchange membrane fuel cells(PEMFCs).However,their c... Platinum(Pt)-based materials are still the most efficient and practical catalysts to drive the sluggish kinetics of cathodic oxygen reduction reaction(ORR)in proton exchange membrane fuel cells(PEMFCs).However,their catalysis and stability performance still need to be further improved in terms of corrosion of both carbon support and Pt catalyst particles as well as Pt loading reduction.Based on the developed synthetic strategies of alloying/nanostructuring Pt particles and modifying/innovating supports in developing conventional Pt-based catalysts,Pt single-atom catalysts(Pt SACs)as the recently burgeoning hot materials with a potential to achieve the maximum utilization of Pt are comprehensively reviewed in this paper.The design thoughts and synthesis of various isolated,alloyed,and nanoparticlecontained Pt SACs are summarized.The single-atomic Pt coordinating with non-metals and alloying with metals as well as the metal-support interactions of Pt single-atoms with carbon/non-carbon supports are emphasized in terms of the ORR activity and stability of the catalysts.To advance further research and development of Pt SACs for viable implementation in PEMFCs,various technical challenges and several potential research directions are outlined. 展开更多
关键词 oxygen reduction electrocatalysis Pt singleatom catalysts conventional Pt-based catalysts design thoughts and synthesis metal-support interactions
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Fullerenes and derivatives as electrocatalysts: Promises and challenges
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作者 Kun Guo Ning Li +1 位作者 Lipiao Bao Xing Lu 《Green Energy & Environment》 SCIE EI CAS CSCD 2024年第1期7-27,共21页
Carbon-based metal-free nanomaterials are promising alternatives to precious metals as electrocatalysts of key energy storage and conversion technologies.Of paramount significance are the establishment of design princi... Carbon-based metal-free nanomaterials are promising alternatives to precious metals as electrocatalysts of key energy storage and conversion technologies.Of paramount significance are the establishment of design principles by understanding the catalytic mechanisms and identifying the active sites.Distinct from sp2-conjugated graphene and carbon nanotube,fullerene possesses unique characteristics that are growingly being discovered and exploited by the electrocatalysis community.For instance,the well-defined atomic and molecular structures,the good electron affinity to tune the electronic structures of other substances,the intermolecular self-assembly into superlattices,and the on-demand chemical modification have endowed fullerene with incomparable advantages as electrocatalysts that are otherwise not applicable to other carbon ma-terials.As increasing studies are being reported on this intriguing topic,it is necessary to provide a state-of-the-art overview of the recent progress.This review takes such an initiative by summarizing the promises and challenges in the electrocatalytic applications of fullerene and its derivatives.The content is structured according to the composition and structure of fullerene,including intact fullerene(e.g.,fullerene composite and superlattices)and fullerene derivatives(e.g.,doped,endohedral,and disintegrated fullerene).The synthesis,characterization,catalytic mechanisms,and deficiencies of these fullerene-based materials are explicitly elaborated.We conclude it by sharing our perspectives on the key aspects that future efforts shall consider. 展开更多
关键词 FULLERENE Fullerene derivative Metal-free catalyst Structural defect ELECTROcatalyst
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Efficient Direct Decomposition of NO over La_(0.8)A_(0.2)NiO_(3)(A=K, Ba, Y) Catalysts under Microwave Irradiation
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作者 王浩 ZHAO Zijian +1 位作者 DUAN Xinghui ZHOU Shijia 《Journal of Wuhan University of Technology(Materials Science)》 SCIE EI CAS CSCD 2024年第1期17-23,共7页
La_(0.8)A_(0.2)NiO_(3) (A=K,Ba,Y) catalysts supported on the microwave-absorbing ceramic heating carrier were prepared by the sol-gel method.The crystalline phase and the catalytic activity of the La_(0.8)A_(0.2)NiO_(... La_(0.8)A_(0.2)NiO_(3) (A=K,Ba,Y) catalysts supported on the microwave-absorbing ceramic heating carrier were prepared by the sol-gel method.The crystalline phase and the catalytic activity of the La_(0.8)A_(0.2)NiO_(3)catalysts were characterized by XRD and H_(2) temperature-programmed reduction (TPR).The effects of reaction temperature,oxygen concentration,and gas flow rate on the direct decomposition of nitric oxide over the synthesized catalysts were studied under microwave irradiation (2.45 GHz).The XRD results indicated that the La_(0.8)A_(0.2)NiO_(3) catalysts formed an ABO_(3) perovskite structure,and the H_(2)-TPR results revealed that the relative reducibility of the catalysts increased in the order of La_(0.8)K_(0.2)NiO_(3)>La_(0.8)Ba_(0.2)NiO_(3)>La_(0.8)Y_(0.2)Ni O_(3).Under microwave irradiation,the highest NO conversion amounted to 98.9%,which was obtained with the La_(0.8)K_(0.2)NiO_(3) catalyst at 400℃.The oxygen concentration did not inhibit the NO decomposition on the La_(0.8)A_(0.2)NiO_(3) catalysts,thus the N_(2) selectivity exceeded 99.8%under excess oxygen at 550℃.The NOconversion of the La_(0.8)A_(0.2)NiO_(3) catalysts decreased linearly with the increase in the gas flow rate. 展开更多
关键词 microwave catalysis direct decomposition of NO microwave-absorbing heating ceramics perovskite catalyst
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Single-atom catalysts for the electrochemical reduction of carbon dioxide into hydrocarbons and oxygenates
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作者 Karl Adrian Gandionco Juwon Kim +2 位作者 Lieven Bekaert Annick Hubin Jongwoo Lim 《Carbon Energy》 SCIE EI CAS CSCD 2024年第3期64-117,共54页
The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic ... The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic material and renewable energy-generated electricity drive the conversion of carbon dioxide into high-value chemicals and carbon-neutral fuels.Over the past few years,single-atom catalysts have been intensively studied as they could provide near-unity atom utilization and unique catalytic performance.Single-atom catalysts have become one of the state-of-the-art catalyst materials for the electrochemical reduction of carbon dioxide into carbon monoxide.However,it remains a challenge for single-atom catalysts to facilitate the efficient conversion of carbon dioxide into products beyond carbon monoxide.In this review,we summarize and present important findings and critical insights from studies on the electrochemical carbon dioxide reduction reaction into hydrocarbons and oxygenates using single-atom catalysts.It is hoped that this review gives a thorough recapitulation and analysis of the science behind the catalysis of carbon dioxide into more reduced products through singleatom catalysts so that it can be a guide for future research and development on catalysts with industry-ready performance for the electrochemical reduction of carbon dioxide into high-value chemicals and carbon-neutral fuels. 展开更多
关键词 ELECTROCATALYSIS electrochemical CO_(2)reduction hydrocarbons OXYGENATES single-atom catalysts
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Boosting Fischer-Tropsch Synthesis via Tuning of N Dopants in TiO_(2)@CN-Supported Ru Catalysts
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作者 Xincheng Li Yunhao Liu +10 位作者 Dejian Zhao Shuaishuai Lyu Jingwei Ye Xiaoshen Li Peipei Wu Ye Tian Yingtian Zhang Tong Ding Song Song Qingpeng Cheng Xingang Li 《Transactions of Tianjin University》 EI CAS 2024年第1期90-102,共13页
Nitrogen(N)-doped carbon materials as metal catalyst supports have attracted signifi cant attention,but the eff ect of N dopants on catalytic performance remains unclear,especially for complex reaction processes such ... Nitrogen(N)-doped carbon materials as metal catalyst supports have attracted signifi cant attention,but the eff ect of N dopants on catalytic performance remains unclear,especially for complex reaction processes such as Fischer-Tropsch synthesis(FTS).Herein,we engineered ruthenium(Ru)FTS catalysts supported on N-doped carbon overlayers on TiO_(2)nanoparticles.By regulating the carbonization temperatures,we successfully controlled the types and contents of N dopants to identify their impacts on metal-support interactions(MSI).Our fi ndings revealed that N dopants establish a favorable surface environment for electron transfer from the support to the Ru species.Moreover,pyridinic N demonstrates the highest electron-donating ability,followed by pyrrolic N and graphitic N.In addition to realizing excellent catalytic stability,strengthening the interaction between Ru sites and N dopants increases the Ru^(0)/Ru^(δ+)ratios to enlarge the active site numbers and surface electron density of Ru species to enhance the strength of adsorbed CO.Consequently,it improves the catalyst’s overall performance,encompassing intrinsic and apparent activities,as well as its ability for carbon chain growth.Accordingly,the as-synthesized Ru/TiO_(2)@CN-700 catalyst with abundant pyridine N dopants exhibits a superhigh C_(5+)time yield of 219.4 mol CO/(mol Ru·h)and C_(5+)selectivity of 85.5%. 展开更多
关键词 Fischer-Tropsch synthesis N-doped carbon materials Ruthenium catalyst Pyridinic N Metal-N interaction
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Strong synergy between physical and chemical properties:Insight into optimization of atomically dispersed oxygen reduction catalysts
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作者 Yifan Zhang Linsheng Liu +4 位作者 Yuxuan Li Xueqin Mu Shichun Mu Suli Liu Zhihui Dai 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第4期36-49,共14页
Atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utiliz... Atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utilization and exceptional catalytic functionality.Furthermore,accurately controlling atomic physical properties including spin,charge,orbital,and lattice degrees of atomically dispersed catalysts can realize the optimized chemical properties including maximum atom utilization efficiency,homogenous active centers,and satisfactory catalytic performance,but remains elusive.Here,through physical and chemical insight,we review and systematically summarize the strategies to optimize atomically dispersed ORR catalysts including adjusting the atomic coordination environment,adjacent electronic orbital and site density,and the choice of dual-atom sites.Then the emphasis is on the fundamental understanding of the correlation between the physical property and the catalytic behavior for atomically dispersed catalysts.Finally,an overview of the existing challenges and prospects to illustrate the current obstacles and potential opportunities for the advancement of atomically dispersed catalysts in the realm of electrocatalytic reactions is offered. 展开更多
关键词 Atomically dispersed catalysts Coordination environment Electronic orbitals Inter-site distance effect Oxygen reduction reaction
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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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A Review on Engineering Transition Metal Compound Catalysts to Accelerate the Redox Kinetics of Sulfur Cathodes for Lithium–Sulfur Batteries
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作者 Liping Chen Guiqiang Cao +8 位作者 Yong Li Guannan Zu Ruixian Duan Yang Bai Kaiyu Xue Yonghong Fu Yunhua Xu Juan Wang Xifei Li 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第5期300-332,共33页
Engineering transition metal compounds(TMCs)catalysts with excellent adsorption-catalytic ability has been one of the most effec-tive strategies to accelerate the redox kinetics of sulfur cathodes.Herein,this review f... Engineering transition metal compounds(TMCs)catalysts with excellent adsorption-catalytic ability has been one of the most effec-tive strategies to accelerate the redox kinetics of sulfur cathodes.Herein,this review focuses on engineering TMCs catalysts by cation doping/anion doping/dual doping,bimetallic/bi-anionic TMCs,and TMCs-based heterostructure composites.It is obvious that introducing cations/anions to TMCs or constructing heterostructure can boost adsorption-catalytic capacity by regulating the electronic structure including energy band,d/p-band center,electron filling,and valence state.Moreover,the elec-tronic structure of doped/dual-ionic TMCs are adjusted by inducing ions with different electronegativity,electron filling,and ion radius,resulting in electron redistribution,bonds reconstruction,induced vacancies due to the electronic interaction and changed crystal structure such as lat-tice spacing and lattice distortion.Different from the aforementioned two strategies,heterostructures are constructed by two types of TMCs with different Fermi energy levels,which causes built-in electric field and electrons transfer through the interface,and induces electron redistribution and arranged local atoms to regulate the electronic structure.Additionally,the lacking studies of the three strategies to comprehensively regulate electronic structure for improving catalytic performance are pointed out.It is believed that this review can guide the design of advanced TMCs catalysts for boosting redox of lithium sulfur batteries. 展开更多
关键词 Lithium–sulfur battery Redox kinetic Transition metal compounds catalyst Multiple metals/anions
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Review of Iron-Based Catalysts for Carbon Dioxide Fischer-Tropsch Synthesis
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作者 Ji-Yue Jia Yu-Ling Shan +3 位作者 Yong-Xiao Tuo Hao Yan Xiang Feng De Chen 《Transactions of Tianjin University》 EI CAS 2024年第2期178-197,共20页
Capturing and utilizing CO_(2)from the production process is the key to solving the excessive CO_(2)emission problem. CO_(2)hydrogenation with green hydrogen to produce olefins is an effective and promising way to uti... Capturing and utilizing CO_(2)from the production process is the key to solving the excessive CO_(2)emission problem. CO_(2)hydrogenation with green hydrogen to produce olefins is an effective and promising way to utilize CO_(2)and produce valuable chemicals. The olefins can be produced by CO_(2)hydrogenation through two routes, i.e., CO_(2)-FTS (carbon dioxide Fischer- Tropsch synthesis) and MeOH (methanol-mediated), among which CO_(2)-FTS has significant advantages over MeOH in practical applications due to its relatively high CO_(2)conversion and low energy consumption potentials. However, the CO_(2)-FTS faces challenges of difficult CO_(2)activation and low olefins selectivity. Iron-based catalysts are promising for CO_(2)-FTS due to their dual functionality of catalyzing RWGS and CO-FTS reactions. This review summarizes the recent progress on iron-based catalysts for CO_(2)hydrogenation via the FTS route and analyzes the catalyst optimization from the perspectives of additives, active sites, and reaction mechanisms. Furthermore, we also outline principles and challenges for rational design of high-performance CO_(2)-FTS catalysts. 展开更多
关键词 CO_(2)hydrogenation OLEFINS CO_(2)-FTS Iron-based catalysts
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Advancements in Catalysts for Electrochemical Nitrate Reduction: A Sustainable Approach for Mitigating Nitrate Pollution: A Review
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作者 Gerald D. S. Quoie Jr. Jean Pierre Bavumiragira Varney Kromah 《Modern Research in Catalysis》 2024年第1期1-28,共28页
Nitrate pollution is of great importance in both the environmental and health contexts, necessitating the development of efficient mitigation strategies. This review provides a comprehensive analysis of the many catal... Nitrate pollution is of great importance in both the environmental and health contexts, necessitating the development of efficient mitigation strategies. This review provides a comprehensive analysis of the many catalysts employed in the electrochemical reduction of nitrate to ammonia, and presents a viable environmentally friendly approach to address the issue of nitrate pollution. Hence, the electrochemical transformation of nitrate to ammonia serves the dual purpose of addressing nitrate pollution in water bodies, and is a useful agricultural resource. This review examines a range of catalyst materials such as noble and non-noble metals, metal oxides, carbon-based materials, nitrogen-doped carbon species, metal complexes, and semiconductor photocatalysts. It evaluates catalytic efficiency, selectivity, stability, and overall process optimization. The performance of catalysts is influenced by various factors, including reaction conditions, catalyst structure, loading techniques, and electrode interfaces. Comparative analysis was performed to evaluate the catalytic activity, selectivity, Faradaic efficiency, current density, stability, and durability of the catalysts. This assessment offers significant perspectives on the structural, compositional, and electrochemical characteristics that affect the efficacy of these catalysts, thus informing future investigations and advancements in this domain. In addition to mitigating nitrate pollution, the electrochemical reduction of nitrate to ammonia is in line with sustainable agricultural methods, resource conservation, and the utilization of renewable energy resources. This study explores the factors that affect the catalytic efficiency, provides new opportunities to address nitrate pollution, and promotes the development of sustainable environmental solutions. 展开更多
关键词 Nitrate Pollution Electrochemical Reduction AMMONIA Sustainable Farming catalysts
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In situ formation of multiple catalysts for enhancing the hydrogen storage of MgH_(2) by adding porous Ni_(3)ZnC_(0.7)/Ni loaded carbon nanotubes microspheres
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作者 Bing Zhang Xiubo Xie +6 位作者 Yukun Wang Chuanxin Hou Xueqin Sun Yuping Zhang Xiaoyang Yang Ronghai Yu Wei Du 《Journal of Magnesium and Alloys》 SCIE EI CAS CSCD 2024年第3期1227-1238,共12页
MgH_(2) is considered one of the most promising hydrogen storage materials because of its safety,high efficiency,high hydrogen storage quantity and low cost characteristics.But some shortcomings are still existed:high... MgH_(2) is considered one of the most promising hydrogen storage materials because of its safety,high efficiency,high hydrogen storage quantity and low cost characteristics.But some shortcomings are still existed:high operating temperature and poor hydrogen absorption dynamics,which limit its application.Porous Ni_(3)ZnC_(0.7)/Ni loaded carbon nanotubes microspheres(NZC/Ni@CNT)is prepared by facile filtration and calcination method.Then the different amount of NZC/Ni@CNT(2.5,5.0 and 7.5 wt%)is added to the MgH_(2) by ball milling.Among the three samples with different amount of NZC/Ni@CNT(2.5,5.0 and 7.5 wt%),the MgH_(2)-5 wt%NZC/Ni@CNT composite exhibits the best hydrogen storage performances.After testing,the MgH_(2)-5 wt%NZC/Ni@CNT begins to release hydrogen at around 110℃ and hydrogen absorption capacity reaches 2.34 wt%H_(2) at 80℃ within 60 min.Moreover,the composite can release about 5.36 wt%H_(2) at 300℃.In addition,hydrogen absorption and desorption activation energies of the MgH_(2)-5 wt%NZC/Ni@CNT composite are reduced to 37.28 and 84.22 KJ/mol H_(2),respectively.The in situ generated Mg_(2)NiH_(4)/Mg_(2)Ni can serve as a"hydrogen pump"that plays the main role in providing more activation sites and hydrogen diffusion channels which promotes H_(2) dissociation during hydrogen absorption process.In addition,the evenly dispersed Zn and MgZn2 in Mg and MgH_(2) could provide sites for Mg/MgH_(2) nucleation and hydrogen diffusion channel.This attempt clearly proved that the bimetallic carbide Ni_(3)ZnC_(0.7) is a effective additive for the hydrogen storage performances modification of MgH_(2),and the facile synthesis of the Ni_(3)ZnC_(0.7)/Ni@CNT can provide directions of better designing high performance carbide catalysts for improving MgH_(2). 展开更多
关键词 Mg-based hydrogen storage material Ni_(3)ZnC_(0.7)/Ni@CNT particles Ni loaded carbon nanotubes Multiple catalysts.
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Ca and Sr co-doping induced oxygen vacancies in 3DOM La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)catalysts for boosting low-temperature oxidative coupling of methane
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作者 Tongtong Wu Yuechang Wei +5 位作者 Jing Xiong Yitao Yang Zhenpeng Wang Dawei Han Zhen Zhao Jian Liu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第4期331-344,共14页
It is urgent to develop catalysts with application potential for oxidative coupling of methane(OCM)at relatively lower temperature.Herein,three-dimensional ordered macro porous(3 DOM)La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)(... It is urgent to develop catalysts with application potential for oxidative coupling of methane(OCM)at relatively lower temperature.Herein,three-dimensional ordered macro porous(3 DOM)La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)(A_(2)B_(2)O_(7)-type)catalysts with disordered defective cubic fluorite phased structure were successfully prepared by a colloidal crystal template method.3DOM structure promotes the accessibility of the gaseous reactants(O2and CH4)to the active sites.The co-doping of Ca and Sr ions in La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)catalysts improved the formation of oxygen vacancies,thereby leading to increased density of surface-active oxygen species(O_(2)^(-))for the activation of CH4and the formation of C2products(C2H6and C2H4).3DOM La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)catalysts exhibit high catalytic activity for OCM at low temperature.3DOM La1.7Sr0.3Ce1.7Ca0.3O7-δcatalyst with the highest density of O_(2)^(-)species exhibited the highest catalytic activity for low-temperature OCM,i.e.,its CH4conversion,selectivity and yield of C2products at 650℃are 32.2%,66.1%and 21.3%,respectively.The mechanism was proposed that the increase in surface oxygen vacancies induced by the co-doping of Ca and Sr ions boosts the key step of C-H bond breaking and C-C bond coupling in catalyzing low-temperature OCM.It is meaningful for the development of the low-temperature and high-efficient catalysts for OCM reaction in practical application. 展开更多
关键词 3DOM catalysts Ca ions Sr ions Low-temperature oxidative couplingof methane Oxygen vacancies O_(2)^(-) species
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A critical review towards the causes of the iron-based catalysts deactivation mechanisms in the selective oxidation of hydrogen sulfide to elemental sulfur from biogas
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作者 Mostafa Tarek Janaina S.Santos +4 位作者 Victor Márquez Mohammad Fereidooni Mohammad Yazdanpanah Supareak Praserthdam Piyasan Praserthdam 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第3期388-411,I0010,共25页
Hydrogen sulfide(H_(2)S) not only presents significant environmental concerns but also induces severe corrosion in industrial equipment,even at low concentrations.Among various technologies,the selective oxidation of ... Hydrogen sulfide(H_(2)S) not only presents significant environmental concerns but also induces severe corrosion in industrial equipment,even at low concentrations.Among various technologies,the selective oxidation of hydrogen sulfide(SOH_(2)S) to elemental sulfur(S) has emerged as a sustainable and environmentally friendly solution.Due to its unique properties,iron oxide has been extensively investigated as a catalyst for SOH_(2)S;however,rapid deactivation has remained a significant drawback.The causes of iron oxide-based catalysts deactivation mechanisms in SOH_(2)S,including sulfur or sulfate deposition,the transformation of iron species,sintering and excessive oxygen vacancy formation,and active site loss,are thoroughly examined in this review.By focusing on the deactivation mechanisms,this review aims to provide valuable insights into enhancing the stability and efficiency of iron-based catalysts for SOH_(2)S. 展开更多
关键词 Selective oxidation of H_(2)S Iron-based catalysts Mechanism of deactivation Sulfur or sulfate deposition Transformation of iron species SINTERING SDG 7
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Designing Oxide Catalysts for Oxygen Electrocatalysis: Insights from Mechanism to Application 被引量:1
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作者 Ning Han Wei Zhang +7 位作者 Wei Guo Hui Pan Bo Jiang Lingbao Xing Hao Tian Guoxiu Wang Xuan Zhang Jan Fransaer 《Nano-Micro Letters》 SCIE EI CAS CSCD 2023年第10期514-546,共33页
The electrochemical oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) are fundamental processes in a range of energy conversion devices such as fuel cells and metal–air batteries. ORR and OER both hav... The electrochemical oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) are fundamental processes in a range of energy conversion devices such as fuel cells and metal–air batteries. ORR and OER both have significant activation barriers, which severely limit the overall performance of energy conversion devices that utilize ORR/OER. Meanwhile, ORR is another very important electrochemical reaction involving oxygen that has been widely investigated. ORR occurs in aqueous solutions via two pathways: the direct 4-electron reduction or 2-electron reduction pathways from O_(2) to water(H_2O) or from O_(2) to hydrogen peroxide(H_2O_(2)). Noble metal electrocatalysts are often used to catalyze OER and ORR, despite the fact that noble metal electrocatalysts have certain intrinsic limitations, such as low storage. Thus, it is urgent to develop more active and stable low-cost electrocatalysts, especially for severe environments(e.g., acidic media). Theoretically, an ideal oxygen electrocatalyst should provide adequate binding to oxygen species. Transition metals not belonging to the platinum group metal-based oxides are a low-cost substance that could give a d orbital for oxygen species binding. As a result, transition metal oxides are regarded as a substitute for typical precious metal oxygen electrocatalysts. However, the development of oxide catalysts for oxygen reduction and oxygen evolution reactions still faces significant challenges, e.g., catalytic activity, stability, cost, and reaction mechanism. We discuss the fundamental principles underlying the design of oxide catalysts, including the influence of crystal structure, and electronic structure on their performance. We also discuss the challenges associated with developing oxide catalysts and the potential strategies to overcome these challenges. 展开更多
关键词 Oxygen evolution Oxygen reduction Oxide catalysts catalyst design Fuel cell Metal–air batteries
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The role of copper in enhancing the performance of heteronuclear diatomic catalysts for the electrochemical CO_(2)conversion to C_(1) chemicals 被引量:1
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作者 Qi Zhao Rachel Crespo-Otero Devis Di Tommaso 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第10期490-500,I0013,共12页
Diatomic catalysts(DACs)with two adjacent metal atoms supported on graphene can offer diverse functionalities,overcoming the inherent limitations of single atom catalysts(SACs).In this study,density functional theory ... Diatomic catalysts(DACs)with two adjacent metal atoms supported on graphene can offer diverse functionalities,overcoming the inherent limitations of single atom catalysts(SACs).In this study,density functional theory calculations were conducted to investigate the reactivity of the carbon dioxide(CO_(2))reduction reaction(CO_(2)RR)on metal sites of both DACs and SACs,as well as their synergistic effects on activity and selectivity.Calculation of the Gibbs free energies of CO_(2)RR and associated values of the limiting potentials to generate C_(1) products showed that Cu acts as a promoter rather than an active catalytic centre in the catalytic CO_(2)conversion on heteronuclear DACs(CuN_(4)-MN_(4)),improving the catalytic activity on the other metal compared to the related SAC MN_(4).Cu enhances the initial reduction of CO_(2)by promoting orbital hybridization between the key intermediate*COOH 2p-orbitals and the metals 3d-orbitals around the Fermi level.This degree of hybridization in the DACs CuN_(4)-MN_(4) decreases from Fe to Co,Ni,and Zn.Our work demonstrates how Cu regulates the CO_(2)RR performance of heteronuclear DACs,offering an effective approach to designing practical,stable,and high-performing diatomic catalysts for CO_(2)electroreduction. 展开更多
关键词 Electrocatalytic CO_(2)reduction Single atom catalysts Diatomic catalysts Graphene Density functional theory calculations
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Aqueous Zinc Batteries with Ultra‑Fast Redox Kinetics and High Iodine Utilization Enabled by Iron Single Atom Catalysts 被引量:2
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作者 Xueya Yang Huiqing Fan +3 位作者 Fulong Hu Shengmei Chen Kang Yan Longtao Ma 《Nano-Micro Letters》 SCIE EI CAS CSCD 2023年第8期368-380,共13页
Rechargeable aqueous zinc iodine(ZnǀǀI_(2))batteries have been promising energy storage technologies due to low-cost position and constitutional safety of zinc anode,iodine cathode and aqueous electrolytes.Whereas,on ... Rechargeable aqueous zinc iodine(ZnǀǀI_(2))batteries have been promising energy storage technologies due to low-cost position and constitutional safety of zinc anode,iodine cathode and aqueous electrolytes.Whereas,on one hand,the low-fraction utilization of electrochemically inert host causes severe shuttle of soluble polyiodides,deficient iodine utilization and sluggish reaction kinetics.On the other hand,the usage of high mass polar electrocatalysts occupies mass and volume of electrode materials and sacrifices device-level energy density.Here,we propose a“confinement-catalysis”host composed of Fe single atom catalyst embedding inside ordered mesoporous carbon host,which can effectively confine and catalytically convert I_(2)/I^(−)couple and polyiodide intermediates.Consequently,the cathode enables the high capacity of 188.2 mAh g^(−1)at 0.3 A g^(−1),excellent rate capability with a capacity of 139.6 mAh g^(−1)delivered at high current density of 15 A g^(−1)and ultra-long cyclic stability over 50,000 cycles with 80.5%initial capacity retained under high iodine loading of 76.72 wt%.Furthermore,the electrocatalytic host can also accelerate the I^(+)↔I_(2)conversion.The greatly improved electrochemical performance originates from the modulation of physicochemical confinement and the decrease of energy barrier for reversible I−/I_(2)and I_(2)/I^(+)couples,and polyiodide intermediates conversions. 展开更多
关键词 Aqueous zinc batteries Iodine reduction reaction Fe single atom catalysts
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High H_(2) selective performance of Ni-Fe-Ca/H-Al catalysts for steam reforming of biomass and plastic 被引量:2
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作者 Jin Deng Lingshuai Meng +4 位作者 Duo Ma Yujie Zhou Xianyang Wang Xiaodong Luo Shenfu Yuan 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第5期215-227,I0006,共14页
The development of a selective catalyst for the conversion of biomass and plastics into H2by steam reforming can combat the energy crisis and global warming.In this work,support Ni-Fe-Ca/H-Al bifunctional catalysts we... The development of a selective catalyst for the conversion of biomass and plastics into H2by steam reforming can combat the energy crisis and global warming.In this work,support Ni-Fe-Ca/H-Al bifunctional catalysts were prepared by loading Ni and Fe into pretreatment CaO/Al_(2)O_(3)(Ca/H-Al)carriers and showed high catalytic activity for the steam reforming of biomass and plastic.Moreover,the idea of bidirectional degradation was exploited to strengthen the pyrolysis of plastic with a high H/C and biomass with a high O/C.Interestingly,the products presented high H2selective(1302.10 m L/g)and low CO_(2)yield(120.23 m L/g)in 7Ni-5Fe-Ca/H-Al(2:4)catalyst compared with current reports.Here,the abundant oxygen vacancies(Ov)in the H-Al carrier exhibited an electron-deficient nature,providing active sites for anchoring Ni O.Meanwhile,Ni O interacted with Ca_(2)Fe_(2)O_(5)to produce more defective Ovsites,which stabilized the NiO particles in the 7Ni-5Fe-Ca/H-Al(2:4)catalyst,and the interaction between the catalyst and the carrier was enhanced,leading to the reduction of weakly basic sites,this property promoted the strong adsorption of CO_(2)and H2O by the catalyst,contributing to the enhancement of efficient steam conversion and the promotion of conversion of by-products to H2.Notably,7Ni-5Fe-Ca/H-Al(2:4)catalysts maintained structural integrity after regeneration and exhibited excellent regenerability in H2selection and CO_(2)adsorption.The work provides a new idea for the study of efficient H2production from steam reforming of biomass and plastics. 展开更多
关键词 Biomass and plastic Pyrolysis Steam reforming Ni-Fe-Ca/H-Al catalyst H_(2)selective
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Separation of Pd and Pt from highly acidic leach liquor of spent automobile catalysts with monothio-Cyanex 272 and trioctylamine 被引量:1
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作者 Junlian Wang Lu Liu +5 位作者 Wen Xu Hui Liu Guodong Xu Kun Huang Fengshan Yu Guoyong Huang 《International Journal of Minerals,Metallurgy and Materials》 SCIE EI CAS CSCD 2023年第5期877-885,共9页
Platinum group metals(PGMs),especially Pd,Pt,and Rh,have drawn great attention due to their unique features.Direct separation of Pd and Pt from highly acidic automobile catalyst leach liquors is disturbed by various f... Platinum group metals(PGMs),especially Pd,Pt,and Rh,have drawn great attention due to their unique features.Direct separation of Pd and Pt from highly acidic automobile catalyst leach liquors is disturbed by various factors.This work investigates the effect of various parameters including the acidity,extractant concentration,phase ratio A/O,and diluents on the Pd and Pt extraction and their stripping behaviors.The results show that the Pd and Pt are successfully separated from simulated leach liquor of spent automobile catalysts with monothioCyanex 272 and trioctylamine(TOA).Monothio-Cyanex 272 shows strong extractability and specific selectivity for Pd,and only one single stage is needed to recover more than 99.9% of Pd,leaving behind all the Pt,Rh,and base metals of Fe,Mg,Ce,Ni,Cu,and Co in the raffinate.The loaded Pd is efficiently stripped by acidic thiourea solutions.TOA shows strong extractability for Pt and Fe at acidity of 6 mol·L^(–1) HCl.More than 99.9% of Pt and all of the Fe are extracted into the organic phase after two stages of countercurrent extraction.Diluted HCl easily scrubs the loaded base metals(Fe,Cu,and Co).The loaded Pt is efficiently stripped by 1.0 mol·L^(–1) thiourea and 0.05–0.1 mol·L^(–1) Na OH solutions.Monothio-Cyanex 272 and TOA can realize the separation of Pd and Pt from highly acidic leach liquor of spent automobile catalysts. 展开更多
关键词 platinum group metals spent automobile catalysts extraction SEPARATION high chloride media
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光学体表成像设备Catalyst的故障维修案例及日常保养方法
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作者 彭旭东 张俞 +1 位作者 何垠波 李光俊 《中国医疗设备》 2024年第4期169-173,180,共6页
本文介绍了光学体表成像设备Catalyst HD的工作原理,以及处理常见的硬件和软件故障的方法,并提供了日常维护保养方法。其中,对于硬件故障,利用Catalyst HD系统的MutilZsn软件来判断Catalyst投影器和摄像头故障,对于软件故障方面,探讨了C... 本文介绍了光学体表成像设备Catalyst HD的工作原理,以及处理常见的硬件和软件故障的方法,并提供了日常维护保养方法。其中,对于硬件故障,利用Catalyst HD系统的MutilZsn软件来判断Catalyst投影器和摄像头故障,对于软件故障方面,探讨了Catalyst HD系统在医用直线加速器上常见的Authorization Pending联锁问题的触发原因。本文为科室更好地开展光学体表引导放疗技术,高效地运用好设备提供参考意见。 展开更多
关键词 光学体表引导放射治疗 catalyst 故障维修 维护保养
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Recent advances in regulating the performance of acid oxygen reduction reaction on carbon-supported non-precious metal single atom catalysts 被引量:1
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作者 Yanqiu Wang Jiayu Hao +6 位作者 Yang Liu Min Liu Kuang Sheng Yue Wang Jun Yang Jie Li Wenzhang Li 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第1期601-616,I0015,共17页
Developing high performance and low-cost catalysts for oxygen reduction reaction(ORR)in challenging acid condition is vital for proton-exchange-membrane fuel cells(PEMFCs).Carbon-supported nonprecious metal single ato... Developing high performance and low-cost catalysts for oxygen reduction reaction(ORR)in challenging acid condition is vital for proton-exchange-membrane fuel cells(PEMFCs).Carbon-supported nonprecious metal single atom catalysts(SACs)have been identified as potential catalysts in the field.Great advance has been obtained in constructing diverse active sites of SACs for improving the performance and understanding the fundamental principles of regulating acid ORR performance.However,the ORR performance of SACs is still unsatisfactory.Importantly,microenvironment adjustment of SACs offers chance to promote the performance of acid ORR.In this review,acid ORR mechanism,attenuation mechanism and performance improvement strategies of SACs are presented.The strategies for promoting ORR activity of SACs include the adjustment of center metal and its microenvironment.The relationship of ORR performance and structure is discussed with the help of advanced experimental investigations and theoretical calculations,which will offer helpful direction for designing advanced SACs for ORR. 展开更多
关键词 Oxygen reduction reaction Single atom catalysts Microenvironment of center metal Regulation of center metal atoms Electron structure Proton-exchange-membrane fuel cells
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