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Comprehensive understanding of the thriving electrocatalytic nitrate/nitrite reduction to ammonia under ambient conditions
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作者 Xinying Zhao Yuzhuo Jiang +5 位作者 Mengfan Wang Yunfei Huan Qiyang Cheng Yanzheng He Tao Qian Chenglin Yan 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第5期459-483,共25页
Ammonia(NH_(3))is a multifunctional compound that is an important feedstock for the agricultural and pharmaceutical industries and attractive energy storage medium.At present,NH_(3)synthesis is highly dependent on the... Ammonia(NH_(3))is a multifunctional compound that is an important feedstock for the agricultural and pharmaceutical industries and attractive energy storage medium.At present,NH_(3)synthesis is highly dependent on the conventional Haber–Bosch process that operates under harsh conditions,which consumes large quantities of fossil fuels and releases a large amount of carbon dioxide.As an alternative,electrosynthesis is a prospective method for producing NH_(3)under normal temperature and pressure conditions.Although electrocatalytic nitrogen reduction to ammonia has attracted considerable attentions,the low solubility of N_(2)and high N≡N cracking energy render the achievements of high NH_(3) yield rate and Faradaic efficiency difficult.Nitrate and nitrite(NO_(x)^(-))are common N-containing pollutants.Due to their high solubilities and low dissociation energy of N=O,NO_(x)^(-)−are ideal raw materials for NH_(3) production.Therefore,electrocatalytic NO_(x)^(-)−reduction to NH_(3)(eNO_(x)RR)is a prospective strategy to simultaneously realise environmental protection and NH_(3) synthesis.This review offers a comprehensive understanding of the thriving eNO_(x)RR under ambient conditions.At first,the popular theory and mechanism of eNO_(x)RR and a summary of the measurement system and evaluation criteria are introduced.Thereafter,various strategies for developing NO_(x)−reduction catalysts are systematically presented and discussed.Finally,the challenges and possible prospects of electrocatalytic NO_(x)^(-1) reduction are outlined to facilitate energy-saving and environmentally friendly large-scale synthesis of NH_(3) in the future. 展开更多
关键词 electrocatalytic nitrate reduction electrocatalytic nitrite reduction Ammonia synthesis Pollutant removal ELECTROSYNTHESIS
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Towards a new avenue for rapid synthesis of electrocatalytic electrodes via laser-induced hydrothermal reaction for water splitting
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作者 Yang Sha Menghui Zhu +6 位作者 Kun Huang Yang Zhang Francis Moissinac Zhizhou Zhang Dongxu Cheng Paul Mativenga Zhu Liu 《International Journal of Extreme Manufacturing》 SCIE EI CAS CSCD 2024年第1期340-351,共12页
Electrochemical production of hydrogen from water requires the development ofelectrocatalysts that are active,stable,and low-cost for water splitting.To address these challenges,researchers are increasingly exploring ... Electrochemical production of hydrogen from water requires the development ofelectrocatalysts that are active,stable,and low-cost for water splitting.To address these challenges,researchers are increasingly exploring binder-free electrocatalytic integratedelectrodes (IEs) as an alternative to conventional powder-based electrode preparation methods,for the former is highly desirable to improve the catalytic activity and long-term stability for large-scale applications of electrocatalysts.Herein,we demonstrate a laser-inducedhydrothermal reaction (LIHR) technique to grow NiMoO4nanosheets on nickel foam,which is then calcined under H2/Ar mixed gases to prepare the IE IE-NiMo-LR.This electrode exhibits superior hydrogen evolution reaction performance,requiring overpotentials of 59,116 and143 mV to achieve current densities of 100,500 and 1000 mA·cm-2.During the 350 h chronopotentiometry test at current densities of 100 and 500 m A·cm-2,the overpotentialremains essentially unchanged.In addition,NiFe-layered double hydroxide grown on Ni foam is also fabricated with the same LIHR method and coupled with IE-NiMo-IR to achieve water splitting.This combination exhibits excellent durability under industrial current density.The energy consumption and production efficiency of the LIHR method are systematicallycompared with the conventional hydrothermal method.The LIHR method significantly improves the production rate by over 19 times,while consuming only 27.78%of the total energy required by conventional hydrothermal methods to achieve the same production. 展开更多
关键词 electrocatalytic electrode laser-induced hydrothermal reaction NiFe layered double hydroxides hydrogen evolution reaction water splitting energy consumption production rate
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Cu-based materials for electrocatalytic CO_(2) to alcohols:Reaction mechanism,catalyst categories,and regulation strategies
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作者 Yaru Lei Yaxin Niu +8 位作者 Xiaolong Tang Xiangtao Yu Xiubing Huang Xiaoqiu Lin Honghong Yi Shunzheng Zhao Jiaying Jiang Jiyue Zhang Fengyu Gao 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第10期593-611,I0013,共20页
Electrocatalytic CO_(2) reduction reaction(CO_(2)RR)technology,which enables carbon capture storage and resource utilization by reducing CO_(2) to valuable chemicals or fuels,has become a global research hotspot in re... Electrocatalytic CO_(2) reduction reaction(CO_(2)RR)technology,which enables carbon capture storage and resource utilization by reducing CO_(2) to valuable chemicals or fuels,has become a global research hotspot in recent decades.Among the many products of CO_(2)RR(carbon monoxide,acids,aldehydes and alcohols,olefins,etc.),alcohols(methanol,ethanol,propanol,etc.)have a higher market value and energy density,but it is also more difficult to produce.Copper is known to be effective in catalyzing CO_(2) to high valueadded alcohols,but with poor selectivity.The progress of Cu-based catalysts for the selective generation of alcohols,including copper oxides,bimetals,single atoms and composites is reviewed.Meanwhile,to improve Cu-based catalyst activity and modulate product selectivity,the modulation strategies are straighten out,including morphological regulation,crystalline surface,oxidation state,as well as elemental doping and defect engineering.Based on the research progress of electrocatalytic CO_(2) reduction for alcohol production on Cu-based materials,the reaction pathways and the key intermediates of the electrocatalytic CO_(2)RR to methanol,ethanol and propanol are summarized.Finally,the problems of traditional electrocatalytic CO_(2)RR are introduced,and the future applications of machine learning and theoretical calculations are prospected.An in-depth discussion and a comprehensive review of the reaction mechanism,catalyst types and regulation strategies were carried out with a view to promoting the development of electrocatalytic CO_(2)RR to alcohols. 展开更多
关键词 electrocatalytic CO_(2)RR Cu-based catalyst ALCOHOLS Reaction mechanism Regulation strategies
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Microfluidic-oriented synthesis of enriched iridium nanodots/carbon architecture for robust electrocatalytic nitrogen fixation
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作者 Hengyuan Liu Xingjiang Wu +2 位作者 Yuhao Geng Xin Li Jianhong Xu 《Green Energy & Environment》 SCIE EI CAS CSCD 2024年第3期544-555,共12页
Electrocatalytic nitrogen reduction reaction(NRR)is considered as a promising candidate to achieve ammonia synthesis because of clean electric energy,moderate reaction condition,safe operating process and harmless by-... Electrocatalytic nitrogen reduction reaction(NRR)is considered as a promising candidate to achieve ammonia synthesis because of clean electric energy,moderate reaction condition,safe operating process and harmless by-products.However,the chemical inertness of nitrogen and poor activated capacity on catalyst surface usually produce low ammonia yield and faradic efficiency.Herein,the microfluidic technology is proposed to efficiently fabricate enriched iridium nanodots/carbon architecture.Owing to in-situ co-precipitation reaction and microfluidic manipulation,the iridium nanodots/carbon nanomaterials possess small average size,uniform dispersion,high conductivity and abundant active sites,producing good proton activation and rapid electrons transmission and moderate adsorption/desorption capacity.As a result,the as-prepared iridium nanodots/carbon nanomaterials realize large ammonia yield of 28.73 μg h^(-1) cm^(-2) and faradic efficiency of 9.14%in KOH solution.Moreover,the high ammonia yield of 11.21 μg h^(-1) cm^(-2) and faradic efficiency of 24.30%are also achieved in H_(2)SO_(4) solution.The microfluidic method provides a reference for large-scale fabrication of nano-sized catalyst materials,which may accelerate the progress of electrocatalytic NRR in industrialization field. 展开更多
关键词 Iridium nanodots CARBON Microfluidic technology Efficient synthesis electrocatalytic nitrogen fixation
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The Electrocatalytic Performance of Rare Earth Ion Doped Co_(0.2)Ni_(0.8)-MOF-74 Catalyst for Nitrogen Reduction
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作者 YUE Song GONG Lunjun +4 位作者 YANG Tonghui HU Weida LIU Xiaopan GAO Pengzhao XIAO Hanning 《Journal of Wuhan University of Technology(Materials Science)》 SCIE EI CAS CSCD 2024年第6期1337-1347,共11页
We took Co_(0.2)Ni_(0.8)-MOF-74 with bimetallic synergistic effect as the basic material,and selected rare earth ions Ho,Gd,and Er with ion radii close to Co and Ni as the research objects for doping.The influence of ... We took Co_(0.2)Ni_(0.8)-MOF-74 with bimetallic synergistic effect as the basic material,and selected rare earth ions Ho,Gd,and Er with ion radii close to Co and Ni as the research objects for doping.The influence of rare earth ion doping amount and doping type on the eNRR performance of the catalyst was explored.The experimental results show that the ammonia yield rate and Faraday efficiency doped with Co_(0.2)Ni_(0.8)-MOF-0.5Ho are the highest,reaching 1.28×10^(-10)mol·s^(-1)·cm^(-2)/39.8%,which is higher than the1.12×10^(-10)mol·s^(-1)·cm^(-2)/32.2%of Co_(0.2)Ni_(0.8)-MOF-74,and is about 14.3%/23.7%higher than that without doping,respectively.And the stability of Co_(0.2)Ni_(0.8)-MOF-0.5 Ho is good(after 80 hours of continuous testing,the current density did not significantly decrease).This is mainly due to doping,which gives Co_(0.2)Ni_(0.8)-MOF-74 a larger specific surface area and catalytic active sites.The catalyst doped at the same time has more metal cation centers,which increases the electron density of the metal centers and enhances the corresponding eNRR performance. 展开更多
关键词 electrocatalytic nitrogen reduction metal organic framework rare earth ions DOPING
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Accelerating H^(*)desorption of hollow Mo_(2)C nanoreactor via in-situ grown carbon dots for electrocatalytic hydrogen evolution
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作者 Mengmeng Liu Yuanyuan Jiang +3 位作者 Zhuwei Cao Lulu Liu Hong Chen Sheng Ye 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第9期464-471,共8页
Molybdenum carbide(Mo_(2)C)is a promising non-noble metal electrocatalyst with electronic structures similar to Pt for hydrogen evolution reaction(HER).However,strong H^(*)adsorption at the Mo sites hinders the improv... Molybdenum carbide(Mo_(2)C)is a promising non-noble metal electrocatalyst with electronic structures similar to Pt for hydrogen evolution reaction(HER).However,strong H^(*)adsorption at the Mo sites hinders the improvement of HER performance.Here,we synthesized monodisperse hollow Mo_(2)C nanoreactors,in which the carbon dots(CD)were in situ formed onto the surface of Mo_(2)C through carburization reactions.According to finite element simulation and analysis,the CD@Mo_(2)C possesses better mesoscale diffusion properties than Mo_(2)C alone.The optimized CD@Mo_(2)C nanoreactor demonstrates superior HER performance in alkaline electrolyte with a low overpotential of 57 mV at 10 mA cm^(−2),which is better than most Mo_(2)C-based electrocatalysts.Moreover,CD@Mo_(2)C exhibits excellent electrochemical stability during 240 h,confirmed by operando Raman and X-ray diffraction(XRD).Density functional theory(DFT)calculations show that carbon dots cause the d-band center of CD@Mo_(2)C to shift away from Fermi level,promoting water dissociation and the desorption of H^(*).This study provides a reasonable strategy towards high-activity Mo-based HER eletrocatalysts by modulating the strength of Mo–H bonds. 展开更多
关键词 Mo_(2)C nanoreactor Carbon dots H^(*)desorption electrocatalytic hydrogen evolution
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Recent advances in phenazine-linked porous catalysts toward photo/electrocatalytic applications and mechanism
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作者 Yang Liu Yu Zhang +1 位作者 Zhao-Di Yang Liqiang Jing 《Green Energy & Environment》 SCIE EI CAS CSCD 2024年第10期1518-1549,共32页
In recent years,porous organic catalysts have been developed and become research hotspots in photo/electrocatalysis due to their inherent pores,high specific surface area,chemical and thermal stability,and diverse fun... In recent years,porous organic catalysts have been developed and become research hotspots in photo/electrocatalysis due to their inherent pores,high specific surface area,chemical and thermal stability,and diverse functional building blocks.Phenazine-linked organic catalysts,exhibited excellent conjugation,electrical conductivity,chemical,and thermal stability,could bring in N atoms with specific numbers and positions to regulate electron levels,anchor metals,and absorb near-infrared light,which expands solar energy utilization.These advantages of the phenazine-linked catalysts attracted our group and numerous researchers to conduct experimental and computational work on photo/electrocatalytic applications and mechanisms.This review summarizes the recent significant research progress,synthesis methods,photo/electrocatalytic performance,and applications of relative phenazine-linked catalysts.Furthermore,the photo/electrocatalytic mechanism was systematized and summarized by combining experiments and density functional theory calculations simultaneously. 展开更多
关键词 Phenazine-linked porous catalysts Photo/electrocatalytic applications Catalytic mechanism
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Recent Advances of Transition Metal Basic Salts for Electrocatalytic Oxygen Evolution Reaction and Overall Water Electrolysis 被引量:13
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作者 Bingrong Guo Yani Ding +4 位作者 Haohao Huo Xinxin Wen Xiaoqian Ren Ping Xu Siwei Li 《Nano-Micro Letters》 SCIE EI CAS CSCD 2023年第4期238-260,共23页
Electrocatalytic oxygen evolution reaction(OER)has been recognized as the bottleneck of overall water splitting,which is a promising approach for sustainable production of H_(2).Transition metal(TM)hydroxides are the ... Electrocatalytic oxygen evolution reaction(OER)has been recognized as the bottleneck of overall water splitting,which is a promising approach for sustainable production of H_(2).Transition metal(TM)hydroxides are the most conventional and classical non-noble metal-based electrocatalysts for OER,while TM basic salts[M^(2+)(OH)_(2-x)(A_(m^(-))_(x/m),A=CO_(3)^(2−),NO_(3)^(−),F^(−),Cl^(−)]consisting of OH−and another anion have drawn extensive research interest due to its higher catalytic activity in the past decade.In this review,we summarize the recent advances of TM basic salts and their application in OER and further overall water splitting.We categorize TM basic salt-based OER pre-catalysts into four types(CO_(3)^(2−),NO_(3)^(−),F^(−),Cl^(−)according to the anion,which is a key factor for their outstanding performance towards OER.We highlight experimental and theoretical methods for understanding the structure evolution during OER and the effect of anion on catalytic performance.To develop bifunctional TM basic salts as catalyst for the practical electrolysis application,we also review the present strategies for enhancing its hydrogen evolution reaction activity and thereby improving its overall water splitting performance.Finally,we conclude this review with a summary and perspective about the remaining challenges and future opportunities of TM basic salts as catalysts for water electrolysis. 展开更多
关键词 Transition metal basic salts electrocatalytic Oxygen evolution reaction(OER) Overall water electrolysis
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Oxygen-coordinated low-nucleus cluster catalysts for enhanced electrocatalytic water oxidation 被引量:5
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作者 Jiapeng Ji Yunpeng Hou +7 位作者 Shiyu Zhou Tong Qiu Liang Zhang Lu Ma Chao Qian Shaodong Zhou Chengdu Liang Min Ling 《Carbon Energy》 SCIE CSCD 2023年第2期137-147,共11页
The oxygen evolution reaction(OER)activity of single-atom catalysts(SACs)is closely related to the coordination environment of the active site.Oxygencoordinated atomic metal species bring about unique features beyond ... The oxygen evolution reaction(OER)activity of single-atom catalysts(SACs)is closely related to the coordination environment of the active site.Oxygencoordinated atomic metal species bring about unique features beyond nitrogen-coordinated atomic metal species due to the fact that the M-O bond is weaker than the M-N bond.Herein,a series of metal-oxygen-carbon structured low-nucleus clusters(LNCs)are successfully anchored on the surface of multiwalled carbon nanotubes(M-MWCNTs,M=Ni,Co,or Fe)through a foolproof low-temperature gas transfer(300℃)method without any further treatment.The morphology and coordination configuration of the LNCs at the atomic level were confirmed by comprehensive characterizations.The synthetic Ni-MWCNTs electrocatalyst features excellent OER activity and stability under alkaline conditions,transcending the performances of Co-MWCNTs,Fe-MWCNTs and RuO_(2).Density functional theory calculations reveal that the moderate oxidation of low-nucleus Ni clusters changes the unoccupied orbital of Ni atoms,thereby lowering the energy barrier of the OER rate-limiting step and making the OER process more energy-efficient.This study demonstrates a novel versatile platform for large-scale manufacturing of oxygen-coordinated LNC catalysts. 展开更多
关键词 electrocatalytic water oxidation low-nucleus cluster low-temperature gas transfer metal-oxygen-carbon structure
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Identification of Dynamic Active Sites Among Cu Species Derived from MOFs@CuPc for Electrocatalytic Nitrate Reduction Reaction to Ammonia 被引量:3
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作者 Xue‑Yang Ji Ke Sun +5 位作者 Zhi‑Kun Liu Xinghui Liu Weikang Dong Xintao Zuo Ruiwen Shao Jun Tao 《Nano-Micro Letters》 SCIE EI CAS CSCD 2023年第8期20-34,共15页
Direct electrochemical nitrate reduction reaction(NITRR)is a promising strategy to alleviate the unbalanced nitrogen cycle while achieving the electrosynthesis of ammonia.However,the restructuration of the high-activi... Direct electrochemical nitrate reduction reaction(NITRR)is a promising strategy to alleviate the unbalanced nitrogen cycle while achieving the electrosynthesis of ammonia.However,the restructuration of the high-activity Cu-based electrocatalysts in the NITRR process has hindered the identification of dynamical active sites and in-depth investigation of the catalytic mechanism.Herein,Cu species(single-atom,clusters,and nanoparticles)with tunable loading supported on N-doped TiO_(2)/C are successfully manufactured with MOFs@CuPc precursors via the pre-anchor and post-pyrolysis strategy.Restructuration behavior among Cu species is co-dependent on the Cu loading and reaction potential,as evidenced by the advanced operando X-ray absorption spectroscopy,and there exists an incompletely reversible transformation of the restructured structure to the initial state.Notably,restructured CuN_(4)&Cu_(4) deliver the high NH_(3) yield of 88.2 mmol h^(−1)g_(cata)^(−1) and FE(~94.3%)at−0.75 V,resulting from the optimal adsorption of NO_(3)^(−) as well as the rapid conversion of^(*)NH_(2)OH to^(*)NH_(2) intermediates originated from the modulation of charge distribution and d-band center for Cu site.This work not only uncovers CuN_(4)&Cu_(4) have the promising NITRR but also identifies the dynamic Cu species active sites that play a critical role in the efficient electrocatalytic reduction in nitrate to ammonia. 展开更多
关键词 Metal-organic frameworks Copper phthalocyanine electrocatalytic nitrate reduction reaction
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Highly Selective Electrocatalytic CuEDTA Reduction by MoS_(2) Nanosheets for Efficient Pollutant Removal and Simultaneous Electric Power Output 被引量:1
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作者 Hehe Qin Xinru Liu +2 位作者 Xiangyun Liu Hongying Zhao Shun Mao 《Nano-Micro Letters》 SCIE EI CAS CSCD 2023年第11期61-73,共13页
Electrocatalytic reduction of ethylenediamine tetraacetic acid copper(CuEDTA),a typical refractory heavy metal complexation pollutant,is an environmental benign method that operates at mild condition.Unfortunately,the... Electrocatalytic reduction of ethylenediamine tetraacetic acid copper(CuEDTA),a typical refractory heavy metal complexation pollutant,is an environmental benign method that operates at mild condition.Unfortunately,the selective reduction of CuEDTA is still a big challenge in cathodic process.In this work,we report a MoS_(2) nanosheet/graphite felt(GF)cathode,which achieves an average Faraday efficiency of 29.6%and specific removal rate(SRR)of 0.042 mol/cm^(2)/h for CuEDTA at−0.65 V vs SCE(saturated calomel electrode),both of which are much higher than those of the commonly reported electrooxidation technology-based removal systems.Moreover,a proofof-concept CuEDTA/Zn battery with Zn anode and MoS_(2)/GF cathode is demonstrated,which has bifunctions of simultaneous CuEDTA removal and energy output.This is one of the pioneer studies on the electrocatalytic reduction of heavy metal complex and CuEDTA/Zn battery,which brings new insights in developing efficient electrocatalytic reduction system for pollution control and energy output. 展开更多
关键词 electrocatalytic reduction CuEDTA removal MoS_(2)nanosheet CuEDTA/Zn battery Faraday efficiency
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Intercalation assisted liquid phase production of disulfide zirconium nanosheets for efficient electrocatalytic dinitrogen reduction to ammonia
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作者 Yangshuo Li Huiyong Wang +5 位作者 Bing Chang Yingying Guo Zhiyong Li Shamraiz Hussain Talib Zhansheng Lu Jianji Wang 《Green Energy & Environment》 SCIE EI CAS CSCD 2023年第4期1174-1184,共11页
Disulfide zirconium(ZrS_(2)) is a two-dimensional(2D) transition metal disulfide and has given rise to extensive attention because of its distinctive electronic structure and properties.However,mass production of high... Disulfide zirconium(ZrS_(2)) is a two-dimensional(2D) transition metal disulfide and has given rise to extensive attention because of its distinctive electronic structure and properties.However,mass production of high quality of ZrS_(2)nanosheets to realize their practical application remains a challenge.Here,we have successfully exfoliated the bulk ZrS_(2)powder with the thickness of micron into single and few-layer nanosheets through liquid-phase exfoliation in N-methylpyrrolidone(NMP) assisted via aliphatic amines as intercalators.It is found that the exfoliation yield is as high as 27.3%,which is the record value for the exfoliation of ZrS_(2)nanosheets from bulk ZrS_(2)powder,and 77.1% of ZrS_(2)nanosheets are 2-3 layers.The molecular geometric size and aliphatic amine basicity have important impact on the exfoliation.Furthermore,the ZrS_(2)nanosheets have been used as catalyst in the electrocatalytic dinitrogen reduction with the NH3yield of 57.75 μg h^(-1)mg_(cat.)^(-1),which is twice that by ZrS_(2)nanofibers reported in literature and three times that by the bulk ZrS_(2)powder.Therefore,the liquid phase exfoliation strategy reported here has great potential in mass production of ZrS_(2)nanosheets for high activity electrocatalysis. 展开更多
关键词 Disulfide zirconium Liquid-phase exfoliation Aliphatic amines electrocatalytic dinitrogen reduction AMMONIA
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Metal-organic framework derived NiFe_(2)O_(4)/FeNi_(3)@C composite for efficient electrocatalytic oxygen evolution reaction
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作者 Fangna Dai Zhifei Wang +6 位作者 Huakai Xu Chuanhai Jiang Yuguo Ouyang Chunyu Lu Yuan Jing Shiwei Yao Xiaofei Wei 《International Journal of Minerals,Metallurgy and Materials》 SCIE EI CAS CSCD 2023年第10期1914-1921,共8页
Reducing the cost and improving the electrocatalytic activity are the key to developing high efficiency electrocatalysts for oxygen evolution reaction(OER).Here,bimetallic NiFe-based metal-organic framework(MOF)was pr... Reducing the cost and improving the electrocatalytic activity are the key to developing high efficiency electrocatalysts for oxygen evolution reaction(OER).Here,bimetallic NiFe-based metal-organic framework(MOF)was prepared by solvothermal method,and then used as precursor to prepare NiFe-based MOF-derived materials by pyrolysis.The effects of different metal ratios and pyrolysis temperatures on the sample structure and OER electrocatalytic performance were investigated and compared.The experimental results showed that when the metal molar ratio was Fe:Ni=1:5 and the pyrolysis temperature was 450℃,the sample(FeNi_(5)-MOF-450)exhibits a composite structure of Ni Fe_(2)O_(4)/FeNi_(3)/C and owns the superior electrocatalytic activity in OER.When the current density is 100 mA·cm^(-2),the overpotential of the sample was 377 mV with Tafel slope of 56.2 mV·dec^(-1),which indicates that FeNi_(5)-MOF-450 exhibits superior electrocatalytic performance than the commercial RuO_(2).Moreover,the long-term stability of FeNi_(5)-MOF-450 further promotes its development in OER.This work demonstrated that the regulatory methods such as component optimization can effectively improve the OER catalytic performance of NiFe-based MOF-derived materials. 展开更多
关键词 metal-organic framework derivatives NiFe-based electrocatalysts electrocatalytic performance oxygen evolution reaction
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From kesterite 2D nanosheets to wurtzite 1D nanorods:controllable synthesis of Cu-Zn-Sn-S and their application in electrocatalytic hydrogen evolution
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作者 Yu Li Shuaibing Wang +4 位作者 Jie Chen Ouyang Lin Zhe Yin Chunhe Yang Aiwei Tang 《Journal of Semiconductors》 EI CAS CSCD 2023年第12期104-110,共7页
As typical quarternary copper-based chalcogenides,Cu–Zn–Sn–S nanocrystals(CZTS NCs)have emerged as a newfashioned electrocatalyst in hydrogen evolution reactions(HERs).Oleylamine(OM),a reducing surfactant and solve... As typical quarternary copper-based chalcogenides,Cu–Zn–Sn–S nanocrystals(CZTS NCs)have emerged as a newfashioned electrocatalyst in hydrogen evolution reactions(HERs).Oleylamine(OM),a reducing surfactant and solvent,plays a significant role in the assisting synthesis of CZTS NCs due to the ligand effect.Herein,we adopted a facile one-pot colloidal method for achieving the structure evolution of CZTS NCs from 2D nanosheets to 1D nanorods assisted through the continuous addition of OM.During the process,the mechanism of OM-induced morphology evolution was further discussed.When merely adding pure 1-dodecanethiol(DDT)as the solvent,the CZTS nanosheets were obtained.As OM was gradually added to the reaction,the CZTS NCs began to grow along the sides of the nanosheets and gradually shrink at the top,followed by the formation of stable nanorods.In acidic electrolytic conditions,the CZTS NCs with 1.0 OM addition display the optimal HER activity with a low overpotential of 561 m V at 10 m A/cm^(2) and a small Tafel slope of 157.6 m V/dec compared with other CZTS samples.The enhancement of HER activity could be attributed to the contribution of the synergistic effect of the diverse crystal facets to the reaction. 展开更多
关键词 2D nanosheets 1D nanorods structure evolution Cu-Zn-Sn-S electrocatalytic hydrogen evolution
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Smart Interfacing between Co-Fe Layered Double Hydroxide and Graphitic Carbon Nitride for High-efficiency Electrocatalytic Nitrogen Reduction
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作者 Xiaohui Wu Lu Tang +5 位作者 Yang Si Chunlan Ma Peng Zhang Jianyong Yu Yitao Liu Bin Ding 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2023年第2期62-69,共8页
Bimetallic compounds such as hydrotalcite-type layered double hydroxides(LDHs)are promising electrocatalysts owing to their unique electronic structures.However,their abilities toward nitrogen adsorption and reduction... Bimetallic compounds such as hydrotalcite-type layered double hydroxides(LDHs)are promising electrocatalysts owing to their unique electronic structures.However,their abilities toward nitrogen adsorption and reduction are undermined since the surface-mantled,electronegative-OH groups hinder the charge transfer between transition metal atoms and nitrogen molecules.Herein,a smart interfacing strategy is proposed to construct a coupled heterointerface between LDH and 2D g-C_(3)N_(4),which is proven by density functional theory(DFT)investigations to be favorable for nitrogen adsorption and ammonia desorption compared with neat LDH surface.The interfaced LDH and g-C_(3)N_(4) is further hybridized with a self-standing TiO_(2) nanofibrous membrane(NM)to maximize the interfacial effect owing to its high porosity and large surface area.Profited from the synergistic superiorities of the three components,the LDH@C_(3)N_(4)@TiO_(2) NM delivers superior ammonia yield(2.07×10^(−9) mol s^(−1) cm^(−2))and Faradaic efficiency(25.3%),making it a high-efficiency,noble-metal-free catalyst system toward electrocatalytic nitrogen reduction. 展开更多
关键词 density functional theory electrocatalytic nitrogen reduction graphitic carbon nitride interface engineering layered double hydroxide
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Preparation and application of g-C_3N_4-ZnS-DNA nanocomposite with enhanced electrocatalytic activity 被引量:2
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作者 周鑫 邹菁 +2 位作者 张胜 潘敏 龚晚芸 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2017年第2期287-295,共9页
We successfully designed and prepared a g-C3N4-ZnS-DNA nanocomposite by a simple method and systematically investigated its morphology,microstructure,and electrocatalytic properties.The as-prepared g-C3N4-ZnS-DNA nano... We successfully designed and prepared a g-C3N4-ZnS-DNA nanocomposite by a simple method and systematically investigated its morphology,microstructure,and electrocatalytic properties.The as-prepared g-C3N4-ZnS-DNA nanocomposite possessed the electrocatalytic activity of g-C3N4-ZnS and the conductivity of DNA.The presence of DNA was found to enhance the electrocatalytic response of the nanocomposite towards environmental hormones,e.g.pentachlorophenol and nonylphenol,owing to the interaction between g-C3N4-ZnS and DNA,indicating that a stable nanocomposite was formed.The three components showed synergistic effects during electrocatalysis.Electrochemical impedance spectra indicated that the g-C3N4-ZnS-DNA nanocomposite dramatically facilitated the electron transfer of a modified electrode.The co-doping of g-C3N4 film with ZnS and DNA doubled the electrochemical response of the modified electrode in comparison with that of unmodified g-C3N4 film.The detection limits(3 S/N) of pentachlorophenol and nonylphenol were3.3×10^-9 mol L^-1.Meanwhile,we propose a possible Z-scheme mechanism for electron transfer in the g-C3N4-ZnS-DNA nanocomposite and the possible pentachlorophenol and nonylphenol electrocatalytic oxidation mechanism.The g-C3N4-ZnS-DNA nanocomposite-modified electrode was demonstrated to be effective for electrochemical sensing of trace environmental hormones in water samples. 展开更多
关键词 Graphitic carbon nitride Zinc sulfide DNA NANOCOMPOSITE electrocatalytic activity Environmental hormones
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Electrocatalytic volcano relations:surface occupation effects and rational kinetic models 被引量:1
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作者 Yongting Chen Junxiang Chen Shengli Chen 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2022年第1期2-10,共9页
Electrocatalysis plays a vital role in technologies of energy and environment relevance,such as water electrolysis,fuel cells,synthesis of carbon and nitrogen-based fuels,etc.The volcano relations(VRs)are general and ... Electrocatalysis plays a vital role in technologies of energy and environment relevance,such as water electrolysis,fuel cells,synthesis of carbon and nitrogen-based fuels,etc.The volcano relations(VRs)are general and standard tools for predicting and understanding the activity trends of electrocatalysts.The modern electrocatalytic VRs are generally based on the kinetic models with the maximum free energy(△G^(0)_(max))of reaction steps as the rate-determining term(RDT),in which some important factors that crucially impact the reaction kinetics are missed,for examples,the surface structures and coverages of reaction intermediates and spectators,other free energy demanding steps than that associated with the △G^(0)_(max),and so on.In this perspective,we first give a brief introduction of the theoretical framework of current electrocatalytic VRs and the underlying problems in the oversimplifiedDG0max-based kinetic models,and then provide an account of our effort in constructing more rational VRs for electrocatalytic reactions.We introduce a new theoretical framework of electrocatalytic VRs based on kinetic model with the so-called energetic span(δE)serving as RDT.Since the surface-coverage effects and multiple free energy-demanding steps are considered,the VRs thus obtained show several new features such as strong potential dependence,asymmetric ascending and descending branches,relatively flat tops,and so on.The effectiveness of theδE-based VRs is verified for hydrogen and oxygen electrocatalytic reactions.Finally,research directions to further rationalize the electrocatalytic VRs are discussed. 展开更多
关键词 ELECTROCATALYSIS Volcano relations Energetic span Hydrogen electrocatalytic reaction Oxygen electrocatalytic reaction
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Electrochemically reduced graphene oxide with enhanced electrocatalytic activity toward tetracycline detection 被引量:4
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作者 胥燕燕 高明明 +4 位作者 张国辉 王新华 李佳佳 王曙光 桑元华 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2015年第11期1936-1942,共7页
An electrochemically reduced graphene oxide sample, ERGO_0.8v, was prepared by electrochemical reduction of graphene oxide (GO) at -0.8 V, which shows unique electrocatalytic activity toward tetracycline (TTC) det... An electrochemically reduced graphene oxide sample, ERGO_0.8v, was prepared by electrochemical reduction of graphene oxide (GO) at -0.8 V, which shows unique electrocatalytic activity toward tetracycline (TTC) detection compared to the ERGO-12v (GO applied to a negative potential of-1.2 V), GO, chemically reduced GO (CRGO)-modified glassy carbon electrode (GC) and bare GC electrodes. The redox peaks of TTC on an ERGO-0.8v-modifled glass carbon electrode (GC/ERGO-0.8v) were within 0-0.5 V in a pH 3.0 buffer solution with the oxidation peak current correlating well with TTC concentration over a wide range from 0.1 to 160 mg/L Physical characterizations with Fourier transform infrared (FT-IR), Raman, and X-ray photoelectron spectroscopies (XPS) demonstrated that the oxygen-containing functional groups on GO diminished after the electrochemical reduction at -0.8 V, yet still existed in large amounts, and the defect density changed as new sp2 domains were formed. These changes demonstrated that this adjustment in the number of oxygen-containing groups might be the main factor affecting the electrocatalytic behavior of ERGO. Additionally, the defect density and sp2 domains also exert a profound influence on this behavior. A possible mechanism for the TTC redox reaction at the GC/ERGO-0.8v electrode is also presented. This work suggests that the electrochemical reduction is an effective method to establish new catalytic activities of GO by setting appropriate parameters. 展开更多
关键词 Electrochemically reduced graphene oxide Electrochemical detection Tetracycline electrocatalytic activity Oxygen-containing functional groups
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Fixation of CO_2 by electrocatalytic reduction to synthesis of dimethyl carbonate in ionic liquid using effective silver-coated nanoporous copper composites 被引量:11
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作者 Xuan Yun Wang Su Qin Liu Ke Long Huang Qiu Ju Feng De Lai Ye Bing Liu Jin Long Liu Guan Hua Jin 《Chinese Chemical Letters》 SCIE CAS CSCD 2010年第8期987-990,共4页
With high surface area,open porosity and high efficiency,a catalyst was prepared and firstly employed in electrocatalytic reduction of CO2 and electrosynthesis of dimethyl carbonate(DMC).The electrochemical property... With high surface area,open porosity and high efficiency,a catalyst was prepared and firstly employed in electrocatalytic reduction of CO2 and electrosynthesis of dimethyl carbonate(DMC).The electrochemical property for electrocatalytic reduction of CO2 in ionic liquid was studied by cyclic voltammogram(CV).The effects of various reaction variables like temperature,working potential and cathode materials on the electrocatalytic performance were also investigated.80%yield of DMC was obtained under the optimal reaction conditions. 展开更多
关键词 electrocatalytic Carbon dioxide NANOPOROUS Dimethyl carbonate Ionic liquid
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Preparation and application of pharmaceutical wastewater treatment by praseodymium doped SnO_2/Ti electrocatalytic electrode 被引量:12
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作者 韩国成 刘峥 王永燎 《Journal of Rare Earths》 SCIE EI CAS CSCD 2008年第4期532-537,共6页
Praseodymium was selected as a promoter for SnO2/Ti electrode to improve the electrocatalytic performance by electrodeposition in pharmaceutical wastewater treatment; the micrograph and the structure were characterize... Praseodymium was selected as a promoter for SnO2/Ti electrode to improve the electrocatalytic performance by electrodeposition in pharmaceutical wastewater treatment; the micrograph and the structure were characterized by SEM and XRD. Mixture uniform design was used in the optimization of the electrolytic conditions; mathematical model was established according to the rate of wiping COD off, which revealed the relationship between the current intensity, time of electrolysis, the amount of doped Pr, and the ratio of area (SnOJTi:Al). On the basis of the analysis of the empirical model, the optimized parameters had been obtained; the rate of wiping COD off was up to 94.9%, it decreased from 392 to 20 mg/L. Experimental results showed that the electrocatalytic performance of the electrode doped with Pr was superior for the treatment of pharmaceutical wastewater. 展开更多
关键词 SnO2/Ti electrode electrocatalytic mixture uniform design pharmaceutical wastewater rare earths
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