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Role of methoxy and C_(α)-based substituents in electrochemical oxidation mechanisms and bond cleavage selectivity of β-O-4 lignin model compounds 被引量:1
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作者 Yang Zhou Qiang Zeng +3 位作者 Hongyan He Kejia Wu Fuqiao Liu Xuehui Li 《Green Energy & Environment》 SCIE EI CAS CSCD 2024年第1期114-125,共12页
In order to better understand the specific substituent effects on the electrochemical oxidation process of β-O-4 bond, a series of methoxyphenyl type β-O-4 dimer model compounds with different localized methoxyl gro... In order to better understand the specific substituent effects on the electrochemical oxidation process of β-O-4 bond, a series of methoxyphenyl type β-O-4 dimer model compounds with different localized methoxyl groups, including 2-(2-methoxyphenoxy)-1-phenylethanone, 2-(2-methoxyphenoxy)-1-phenylethanol, 2-(2-methoxyphenoxy)-1-(4-methoxyphenyl)ethanone, 2-(2-methoxyphenoxy)-1-(4-methoxyphenyl)ethanol, 2-(2,6-dimethoxyphenoxy)-1-(4-methoxyphenyl)ethanone, 2-(2,6-dimethoxyphenoxy)-1-(4-methoxyphenyl)ethanol have been selected and their electrochemical properties have been studied experimentally by cyclic voltammetry, and FT-IR spectroelectrochemistry. Combining with electrolysis products distribution analysis and density functional theory calculations, oxidation mechanisms of all six model dimers have been explored. In particular, a total effect from substituents of both para-methoxy(on the aryl ring closing to Cα) and Cα-OH on the oxidation mechanisms has been clearly observed, showing a significant selectivity on the Cα-Cβbond cleavage induced by electrochemical oxidations. 展开更多
关键词 Lignin model compounds β-O-4 dimers electrochemical oxidation oxidation mechanisms Substituent effect
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Electrochemical reduction of carbon dioxide to produce formic acid coupled with oxidative conversion of biomass
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作者 Xi Liu Yifan Wang +2 位作者 Zhiwei Dai Daihong Gao Xuebing Zhao 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第5期705-729,共25页
Electrochemical reduction of CO_(2)(CO_(2)RR)has become a research hot spot in recent years in the context of carbon neutrality.HCOOH is one of the most promising products obtained by electrochemical reduction of CO_(... Electrochemical reduction of CO_(2)(CO_(2)RR)has become a research hot spot in recent years in the context of carbon neutrality.HCOOH is one of the most promising products obtained by electrochemical reduction of CO_(2) due to its high energy value as estimated by market price per energy unit and wide application in chemical industry.Biomass is the most abundant renewable resource in the natural world.Coupling biomass oxidative conversion with CO_(2)RR driven by renewable electricity would well achieve carbon negativity.In this work,we comprehensively reviewed the current research progress on CO_(2)RR to produce HCOOH and coupled system for conversion of biomass and its derivatives to produce value-added products.Sn-and Bi-based electrocatalysts are discussed for CO_(2)RR with regards to the structure of the catalyst and reaction mechanisms.Electro-oxidation reactions of biomass derived sugars,alcohols,furan aldehydes and even polymeric components of lignocellulose were reviewed as alternatives to replace oxygen evolution reaction(OER)in the conventional electrolysis process.It was recommended that to further improve the efficiency of the coupled system,future work should be focused on the development of more efficient and stable catalysts,careful design of the electrolytic cells for improving the mass transfer and development of environment-friendly processes for recovering the formed formate and biomass oxidation products. 展开更多
关键词 electrochemical reduction of CO_(2) Formic acid oxidative conversion of biomass LIGNOCELLULOSE Coupled system
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In-situ oriented oxygen-defect-rich Mn-N-O via nitridation and electrochemical oxidation based on industrial-scale Mn_(2)O_(3) to achieve high-performance aqueous zinc ion battery
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作者 Yao Liu Shuailong Guo +7 位作者 Wei Ling Mangwei Cui Hao Lei Jiaqi Wang Wenzheng Li Qingjiang Liu Lukuan Cheng Yan Huang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第1期11-18,I0001,共9页
As a general problem in the field of batteries,materials produced on a large industrial scale usually possess unsatisfactory electrochemical performances.Among them,manganese-based aqueous rechargeable zinc-ion batter... As a general problem in the field of batteries,materials produced on a large industrial scale usually possess unsatisfactory electrochemical performances.Among them,manganese-based aqueous rechargeable zinc-ion batteries(ARZBs)have been emerging as promising large-scale energy storage systems owing to their high energy densities,low manufacturing cost and intrinsic high safety.However,the direct application of industrial-scale Mn2O3(MO)cathode exhibits poor electrochemical performance especially at high current rates.Herein,a highly reversible Mn-based cathode is developed from the industrial-scale MO by nitridation and following electrochemical oxidation,which triples the ion diffusion rate and greatly promotes the charge transfer.Notably,the cathode delivers a capacity of 161 m Ah g^(-1) at a high current density of 10 A g^(-1),nearly-three times the capacity of pristine MO(60 m Ah g^(-1)).Impressive specific capacity(243.4 m Ah g^(-1))is obtained without Mn^(2+) additive added in the electrolyte,much superior to the pristine MO(124.5 m Ah g^(-1)),suggesting its enhanced reaction kinetics and structural stability.In addition,it possesses an outstanding energy output of 368.4 Wh kg^(-1) at 387.8 W kg^(-1),which exceeds many of reported cathodes in ARZBs,providing new opportunities for the large-scale application of highperformance and low-cost ARZBs. 展开更多
关键词 Aqueous rechargeable zinc-ion battery Mn-based cathode Oxygen defect NITRIDATION electrochemical oxidation
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Synthesis of three-dimensional ordered mesoporous MnO_2 and its catalytic performance in formaldehyde oxidation 被引量:20
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作者 拜冰阳 乔琦 +1 位作者 李俊华 郝吉明 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2016年第1期27-31,共5页
Three-dimensional(3D)ordered mesoporous MnO2 was prepared using KIT-6 mesoporous molecular sieves as a hard template.The material was used for catalytic oxidation of HCHO.The material has high surface areas and the ... Three-dimensional(3D)ordered mesoporous MnO2 was prepared using KIT-6 mesoporous molecular sieves as a hard template.The material was used for catalytic oxidation of HCHO.The material has high surface areas and the mesoporous characteristics of the template,with cubic symmetry(ia3d).It consists of a β-MnO2 crystalline phase corresponding to pyrolusite,with a rutile structure.Transmission electron microscopy and X-ray photoelectron spectroscopy showed that the 3D-MnO2 catalyst has a large number of exposed Mn4+ ions on the(110)crystal plane surfaces,with a lattice spacing of 0.311 nm; this enhances oxidation of HCHO.Complete conversion of HCHO to CO2 and H2O was achieved at 130 °C on 3D-MnO2; the same conversions on α-MnO2 and β-MnO2 nanorods were obtained at 140 and 180 °C,respectively,under the same conditions.The specific mesoporous structure,high specific surface area,and large number of surface Mn4+ ions are responsible for the catalytic activity of 3D-MnO2 in HCHO oxidation. 展开更多
关键词 three-dimensional ordered material Mesoporous structure Manganese oxide FORMALDEHYDE Catalytic oxidation
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Electrochemical oxidation of aniline by a novel Ti/TiO_xH_y/Sb-SnO_2 electrode 被引量:8
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作者 李晓良 徐浩 延卫 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2016年第11期1860-1870,共11页
Electrochemical oxidation of aniline in aqueous solution was investigated over a novel Ti/TiOxHy/Sb-SnO2 electrode prepared by the electrodeposition method.Scanning electron microscopy,X-ray diffraction,and electroche... Electrochemical oxidation of aniline in aqueous solution was investigated over a novel Ti/TiOxHy/Sb-SnO2 electrode prepared by the electrodeposition method.Scanning electron microscopy,X-ray diffraction,and electrochemical measurements were used to characterize its morphology,crystal structure,and electrochemical properties.Removal of aniline by the Ti/TiOxHy/Sb-SnO2electrode was investigated by ultraviolet-Visible spectroscopy and chemical oxygen demand(COD)analysis under different conditions,including current densities,initial concentrations of aniline,pH values,concentrations of chloride ions,and types of reactor.It was found that a higher current density,a lower initial concentration of aniline,an acidic solution,the presence of chloride ions(0.2wt%NaCl),and a three-dimensional(3D) reactor promoted the removal efficiency of aniline.Electrochemical degradation of aniline followed pseudo-first-order kinetics.The aniline(200 mL of 100mg·L-(-1)) and COD removal efficiencies reached 100%and 73.5%,respectively,at a current density of 20 mA·cm-(-2),pH of 7.0,and supporting electrolyte of 0.5 wt%Na2SO4 after 2 h electrolysis in a 3D reactor.These results show that aniline can be significantly removed on the Ti/TiOxHy/Sb-SnO2electrode,which provides an efficient way for elimination of aniline from aqueous solution. 展开更多
关键词 ANILINE Ti/TiOxHy/Sb-SnO2 electrode electrochemical oxidation Chloride ions three-dimensional reactor
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Preparation and Electrochemical Characteristics of Three-dimensional Manganese Oxide Micro-supercapacitor Electrode
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作者 Chun-ming Wen Zhi-yu Wen +1 位作者 Zheng You Xiao-feng Wang 《Chinese Journal of Chemical Physics》 SCIE CAS CSCD 2012年第2期209-213,I0004,共6页
In order to increase the electrode surface area and enhance the charge storage capacity, we study the micro electro mechanical system technology to fabricate three-dimensional high aspect ratio micro-electrode structu... In order to increase the electrode surface area and enhance the charge storage capacity, we study the micro electro mechanical system technology to fabricate three-dimensional high aspect ratio micro-electrode structure based on glass. The anodic constant potential method is employed to deposit manganese oxide as electroactive substances on the micro-electrode surface. Cyclic voltammetry and constant current charge-discharge method are both used to prepare electrode electrochemical performance testing, with a two-dimensional electrode without structure for comparison. Experimental results show that three-dimensional elec- trode structure can effectively enhance the charge storage capacity. At 1.0 mA/cm2 charge- discharge density, the three-dimensional electrode shows a capacitance of 17.88 mF/cm2, seven times higher than the two-dimensional electrode. 展开更多
关键词 Micro-supercapacitor Micro electro mechanical system three-dimensional electrode Manganese oxide
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Study on Methanol Oxidation at Pt and PtRu Electrodes by Combining in situ Infrared Spectroscopy and Differential Electrochemical Mass Spectrometry 被引量:1
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作者 陶骞 陈微 +2 位作者 姚瑶 Ammar Bin Yousaf 陈艳霞 《Chinese Journal of Chemical Physics》 SCIE CAS CSCD 2014年第5期541-547,I0003,共8页
Methanol oxidation reaction (MOR) at Pt and Pt electrode surface deposited with various amounts of Ru (denoted as PtxRuy, nominal coverage y is 0.17, 0.27, and 0.44 ML) in 0.1 mol/L HClO4+0.5 mol/L MeOH has been ... Methanol oxidation reaction (MOR) at Pt and Pt electrode surface deposited with various amounts of Ru (denoted as PtxRuy, nominal coverage y is 0.17, 0.27, and 0.44 ML) in 0.1 mol/L HClO4+0.5 mol/L MeOH has been studied under potentiostatic conditions by in situ FTIR spectroscopy in attenuated-total-reflection con guration and di erential electro-chemical mass spectrometry under controlled flow conditions. Results reveal that (i) CO is the only methanol-related adsorbate observed by IR spectroscopy at all the Pt and PtRu electrodes examined at potentials from 0.3 V to 0.6 V (vs. RHE); (ii) at Pt0.56Ru0.44, two IR bands, one from CO adsorbed at Ru islands and the other from COL at Pt substrate are detected, while at other electrodes, only a single band for COL adsorbed at Pt is observed; (iii) MOR activity decreases in the order of Pt0.73Ru0.27〉Pt0.56Ru0.44〉Pt0.83Ru0.17〉Pt; (iv) at 0.5 V, MOR at Pt0.73Ru0.27 reaches a current e ciency of 50% for CO2 production, the turn-over frequency from CH3OH to CO2 is ca. 0.1 molecule/(site sec). Suggestions for further improving of PtRu catalysts for MOR are provided. 展开更多
关键词 Differential electrochemical mass spectrometry electrochemical in situ infrared spectroscopy Methanol oxidation PtRu electrode Current efficiency
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Sustainable Furfural Biomass Feedstocks Electrooxidation toward Value-Added Furoic Acid with Energy-Saving H_(2) Fuel Production Using Pt-Decorated Co_(3)O_(4) Nanospheres 被引量:1
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作者 Talshyn Begildayeνa Jayaraman Theerthagiri +4 位作者 Seung Jun Lee Ahreum Min Gyeong-Ah Kim Siνakumar Manickam Myong Yong Choi 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2024年第2期350-358,共9页
Here,furfural oxidation was performed to replace the kinetically sluggish O_(2)evolution reaction(OER).Pt-Co_(3)O_(4)nanospheres were developed via pulsed laser ablation in liquid(PLAL)in a single step for the paired ... Here,furfural oxidation was performed to replace the kinetically sluggish O_(2)evolution reaction(OER).Pt-Co_(3)O_(4)nanospheres were developed via pulsed laser ablation in liquid(PLAL)in a single step for the paired electrocatalysis of an H_(2)evolution reaction(HER)and furfural oxidation reaction(FOR).The FOR afforded a high furfural conversion(44.2%)with a major product of 2-furoic acid after a 2-h electrolysis at 1.55 V versus reversible hydrogen electrode in a 1.0-M KOH/50-mM furfural electrolyte.The Pt-Co_(3)O_(4)electrode exhibited a small overpotential of 290 mV at 10 mA cm^(-2).As an anode and cathode in an electrolyzer system,the Pt-Co_(3)O_(4)electrocatalyst required only a small applied cell voltage of~1.83 V to deliver 10 mA cm^(-2),compared with that of the pure water electrolyzer(OER||HER,~1.99 V).This study simultaneously realized the integrated production of energy-saving H_(2)fuel at the cathode and 2-furoic acid at the anode. 展开更多
关键词 biomass conversion electrochemical furfural oxidation overall water splitting Pt-Co_(3)O_(4)electrocatalyst pulsed laser ablation in liquid
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Tuning the reactivity of TiO_(2)layer with uniform distribution of Sub-5 nm Fe_(2)O_(3)particles via in situ voltage-assisted oxidation for robust catalytic reduction
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作者 Nisa Nashrah Abdelkarim Chaouiki +1 位作者 Wail Al Zoubi Young Gun Ko 《Nano Materials Science》 EI CAS CSCD 2024年第2期223-234,共12页
The trade-off between efficiency and stability has limited the application of TiO_(2)as a catalyst due to its poor surface reactivity.Here,we present a modification of a TiO_(2)layer with highly stable Sub-5 nm Fe_(2)... The trade-off between efficiency and stability has limited the application of TiO_(2)as a catalyst due to its poor surface reactivity.Here,we present a modification of a TiO_(2)layer with highly stable Sub-5 nm Fe_(2)O_(3)nanoparticles(NP)by modulating its structure-surface reactivity relationship to attain efficiency-stability balance via a voltage-assisted oxidation approach.In situ simultaneous oxidation of the Ti substrate and Fe precursor using high-energy plasma driven by high voltage resulted in uniform distribution of Fe_(2)O_(3)NP embedded within porous TiO_(2)layer.Comprehensive surface characterizations with density functional theory demonstrated an improved electronic transition in TiO_(2)due to the presence of surface defects from reactive oxygen species and possible charge transfer from Ti to Fe;it also unexpectedly increased the active site in the TiO_(2)layer due to uncoordinated electrons in Sub-5 nm Fe_(2)O_(3)NP/TiO_(2)catalyst,thereby enhancing the adsorption of chemical functional groups on the catalyst.This unique embedded structure exhibited remarkable improvement in reducing 4-nitrophenol to 4-aminophenol,achieving approximately 99%efficiency in 20 min without stability decay after 20 consecutive cycles,outperforming previously reported TiO_(2)-based catalysts.This finding proposes a modified-electrochemical strategy enabling facile construction of TiO_(2)with nanoscale oxides extandable to other metal oxide systems. 展开更多
关键词 Titanium dioxide oxide nanoparticle electrochemical oxidation Surface reactivity Efficiency Stability
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Identification of optimal composition with superior electrochemical properties along the zero Mn^(3+)line in Na_(0.75)(Mn-Al-Ni)O_(2)pseudo ternary system
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作者 Hari Narayanan Vasavan Manish Badole +8 位作者 Samriddhi Saxena Velaga Srihari Asish Kumar Das Pratiksha Gami Neha Dagar Sonia Deswal Pradeep Kumar Himanshu Kumar Poswal Sunil Kumar 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第9期206-216,共11页
Biphasic layered oxide cathodes,known for their superior electrochemical performance,are prime candidates for commercializing in Na-ion batteries.Herein,we unveil a series of P3/P2 monophasic and biphasic Al-substitut... Biphasic layered oxide cathodes,known for their superior electrochemical performance,are prime candidates for commercializing in Na-ion batteries.Herein,we unveil a series of P3/P2 monophasic and biphasic Al-substituted Na_(3/4)Mn_(5-x/8)Al_(2x/8)Ni_(3-x/8)O_(2)layered oxide cathodes that lie along the‘zero Mn^(3+)line’in the Na_(3/4)(Mn-Al-Ni)O_(2)pseudo-ternary system.The structural analysis showed a larger Na^(+)conduction bottleneck area in both P3 and P2 structures with a higher Al3+content,which enhanced their rate performance.In each composition,the P3/P2 biphasic compound with nearly equal fractions of P3 and P2 phases outperformed their monophasic counterparts in almost all electrochemical performance parameters.Operando synchrotron XRD measurements obtained for the monophasic P3 and biphasic P2/P3 samples revealed the absence of the O3 phase during cycling.The high structure stability and faster Na^(+)transport kinetics in the biphasic samples underpins the enhancement of electrochemical properties in the Al-substituted P3/P2 cathodes.These results highlight fixed oxidation state lines as a novel tool to identify and design layered oxide cathodes for Na-ion batteries in pseudo-ternary diagrams involving Jahn-Teller active cations. 展开更多
关键词 Layered oxides Biphasic cathode Operando Synchrotron XRD electrochemical behavior Cyclic performance
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Antagonism effect of residual S triggers the dual-path mechanism for water oxidation
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作者 Li Liu Jinming Cao +5 位作者 Siqi Hu Tinghui Liu Can Xu Wensheng Fu Xinguo Ma Xiaohui Yang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第6期568-579,I0014,共13页
Transition metal chalcogenides(TMCs)are recognized as pre-catalysts,and their(oxy)hydroxides derived from electrochemical reconstruction are the active species in the water oxidation.However,understanding the role of ... Transition metal chalcogenides(TMCs)are recognized as pre-catalysts,and their(oxy)hydroxides derived from electrochemical reconstruction are the active species in the water oxidation.However,understanding the role of the residual chalcogen in the reconstructed layer is lacking in detail,and the corresponding catalytic mechanism remains controversial.Here,taking Cu_(1-x)Co_(x)S as a platform,we explore the regulating effect and existence form of the residual S doped into the reconstructive layer for oxygen evolution reaction(OER),where a dual-path OER mechanism is proposed.First-principles calculations and operando~(18)O isotopic labeling experiments jointly reveal that the residual S in the reconstructive layer of Cu_(1-x)Co_(x)S can wisely balance the adsorbate evolution mechanism(AEM)and lattice oxygen oxidation mechanism(LOM)by activating lattice oxygen and optimizing the adsorption/desorption behaviors at metal active sites,rather than change the reaction mechanism from AEM to LOM.Following such a dual-path OER mechanism,Cu_(0.4)Co_(0.6)S-derived Cu_(0.4)Co_(0.6)OSH not only overcomes the restriction of linear scaling relationship in AEM,but also avoids the structural collapse caused by lattice oxygen migration in LOM,so as to greatly reduce the OER potential and improved stability. 展开更多
关键词 electrochemical reconstruction Adsorbate evolution mechanism Lattice oxygen oxidation mechanism Oxygen evolution reaction Residual sulfur
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Electrochemical behavior of Fe(Ⅲ)in Na_(2)SiO_(3)-SiO_(2)-Fe_(2)O_(3)molten salt
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作者 FENG Sen ZHANG Jun-jie +4 位作者 DIOP Mouhamadou Aziz LIU Ai-min WANG Zhao-wen BOCA Miroslav SHI Zhong-ning 《Journal of Central South University》 SCIE EI CAS CSCD 2024年第9期3024-3033,共10页
The high-temperature requirement for liquid iron smelting via molten oxide electrolysis presents significant challenges.This study investigates the electrochemical reduction of Fe(Ⅲ)in a novel low-temperature electro... The high-temperature requirement for liquid iron smelting via molten oxide electrolysis presents significant challenges.This study investigates the electrochemical reduction of Fe(Ⅲ)in a novel low-temperature electrolyte,Na_(2)SiO_(3)-SiO_(2)-Fe_(2)O_(3),utilizing cyclic voltammetry and square wave voltammetry techniques.The results show that Fe(Ⅲ)reduction occurs in two steps:Fe(Ⅲ)+e^(−)→Fe(Ⅱ),Fe(Ⅱ)+2e^(−)→Fe,and that the redox process of Fe(Ⅲ)/Fe(Ⅱ)at the tungsten electrode is an irreversible reaction controlled by diffusion.The diffusion coefficients of Fe(Ⅲ)in the molten Na_(2)SiO_(3)-SiO_(2)-Fe_(2)O_(3)in the temperature range of 1248–1278 K are between 1.86×10^(−6)cm^(2)/s and 1.58×10^(−4)cm^(2)/s.The diffusion activation energy of Fe(Ⅲ)in the molten salt is 1825.41 kJ/mol.As confirmed by XRD analysis,potentiostatic electrolysis at−0.857 V(vs.O_(2)/O_(complex)^(2-))for 6 h produces metallic iron on the cathode. 展开更多
关键词 molten oxide electrolysis(MOE) electrochemical behavior cyclic voltammetry potentiostatic electrolysis diffusion coefficients Fe(Ⅲ)
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Layer by Layer Self-assembly Fiber-based Flexible Electrochemical Transistor
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作者 谭艳 HAO Panpan +2 位作者 HE Yang ZHU Rufeng 王跃丹 《Journal of Wuhan University of Technology(Materials Science)》 SCIE EI CAS CSCD 2024年第4期937-944,共8页
Poly(3,4-ethylenedioxyethiophene)-polystyrene sulfonic acid(PEDOT:PSS)/polyallyl dimethyl ammonium chloride modified reduced graphene oxide(PDDA-rGO)was layer by layer self-assembled on the cotton fiber.The surface mo... Poly(3,4-ethylenedioxyethiophene)-polystyrene sulfonic acid(PEDOT:PSS)/polyallyl dimethyl ammonium chloride modified reduced graphene oxide(PDDA-rGO)was layer by layer self-assembled on the cotton fiber.The surface morphology and electric property was investigated.The results confirmed the dense membrane of PEDOT:PSS and the lamellar structure of PDDA-rGO on the fibers.It has excellent electrical conductivity and mechanical properties.The fiber based electrochemical transistor(FECTs)prepared by the composite conductive fiber has a maximum output current of 8.7 mA,a transconductance peak of 10 mS,an on time of 1.37 s,an off time of 1.6 s and excellent switching stability.Most importantly,the devices by layer by layer self-assembly technology opens a path for the true integration of organic electronics with traditional textile technologies and materials,laying the foundation for their later widespread application. 展开更多
关键词 layer by layer SELF-ASSEMBLY fiber based organic electrochemical transistor reduced graphene oxide PEDOT:PSS
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Bimetallic CoNi single atoms supported on three-dimensionally ordered mesoporous chromia:highly active catalysts for n-hexane combustion
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作者 Xiuqing Hao Yuxi Liu +4 位作者 Jiguang Deng Lin Jing Jia Wang Wenbo Pei Hongxing Dai 《Green Energy & Environment》 SCIE EI CAS CSCD 2024年第7期1122-1137,共16页
Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile... Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile organic compounds(VOCs).In this work,we prepared the mesoporous chromia-supported bimetallic Co and Ni single-atom(Co_(1)Ni_(1)/meso-Cr_(2)O_(3))and bimetallic Co and Ni nanoparticle(Co_(NP)Ni_(NP)/mesoCr_(2)O_(3))catalysts adopting the one-pot polyvinyl pyrrolidone(PVP)-and polyvinyl alcohol(PVA)-protecting approaches,respectively.The results indicate that the Co_(1)Ni_(1)/meso-Cr_(2)O_(3)catalyst exhibited the best catalytic activity for n-hexane(C_(6)H_(14))combustion(T_(50%)and T_(90%)were 239 and 263℃ at a space velocity of 40,000 mL g^(-1)h^(-1);apparent activation energy and specific reaction rate at 260℃ were 54.7 kJ mol^(-1)and 4.3×10^(-7)mol g^(-1)_(cat)s^(-1),respectively),which was associated with its higher(Cr^(5+)+Cr^(6+))amount,large n-hexane adsorption capacity,and good lattice oxygen mobility that could enhance the deep oxidation of n-hexane,in which Ni_(1) was beneficial for the enhancements in surface lattice oxygen mobility and low-temperature reducibility,while Co_(1) preferred to generate higher contents of the high-valence states of chromium and surface oxygen species as well as adsorption and activation of n-hexane.n-Hexane combustion takes place via the Mars van Krevelen(MvK)mechanism,and its reaction pathways are as follows:n-hexane→olefins or 3-hexyl hydroperoxide→3-hexanone,2-hexanone or 2,5-dimethyltetrahydrofuran→2-methyloxirane or 2-ethyl-oxetane→acrylic acid→CO_x→CO_(2)and H_(2)O. 展开更多
关键词 three-dimensional ordered mesoporous chromium oxide Supported bimetallic single-atom catalyst Cobalt-nickel single atoms n-Hexane combustion Catalytic reaction mechanism
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Self-repairing Al_(2)O_(3)-TiO_(2)coatings fabricated through plasma electrolytic oxidation with various cathodic pulse parameters
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作者 Mehri HASHEMZADEH Keyvan RAEISSI +4 位作者 Fakhreddin ASHRAFIZADEH Frank SIMCHEN Amin HAKIMIZAD Monica SANTAMARIA Thomas LAMPKE 《Transactions of Nonferrous Metals Society of China》 SCIE EI CAS CSCD 2024年第10期3326-3343,共18页
The influence of cathodic pulse parameters was evaluated on plasma electrolytic oxidation(PEO)coatings grown on 7075 aluminum alloy in a silicate-based electrolyte containing potassium titanyl oxalate(PTO)using pulsed... The influence of cathodic pulse parameters was evaluated on plasma electrolytic oxidation(PEO)coatings grown on 7075 aluminum alloy in a silicate-based electrolyte containing potassium titanyl oxalate(PTO)using pulsed bipolar waveforms with various cathodic duty cycles and cathodic current densities.The coatings were characterized by SEM,EDS,and XRD.EIS was applied to investigate the electrochemical properties.It was observed that the increase of cathodic duty cycle and cathodic current density from 20%and 6 A/dm^(2) to 40%and 12 A/dm^(2) enhances the growth rate of the inner layer from 0.22 to 0.75μm/min.Adding PTO into the bath showed a fortifying effect on influence of the cathodic pulse and the mentioned change of cathodic pulse parameters,resulting in an increase of the inner layer growth rate from 0.25 to 1.10μm/min.Based on EDS analysis,Si and Ti were incorporated dominantly in the upper parts of the coatings.XRD technique merely detectedγ-Al_(2)O_(3),and there were no detectable peaks related to Ti and Si compounds.However,the EIS results confirmed that the incorporation of Ti^(4+)into alumina changed the electronic properties of the coating.The coatings obtained from the bath containing PTO using the bipolar waveforms with a cathodic duty cycle of 40%and current density values higher than 6 A/dm^(2) showed highly appropriate electrochemical behavior during 240 d of immersion due to an efficient repairing mechanism.Regarding the effects of studied parameters on the coating properties,the roles of cathodic pulse parameters and PTO in the PEO process were highlighted. 展开更多
关键词 Al2O3−TiO2 coating plasma electrolytic oxidation potassium titanyl oxalate electrochemical impedance spectroscopy
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Comparative structural and electrochemical properties of mixed P2/O′3-layered sodium nickel manganese oxide prepared by sol-gel and electrospinning methods:Effect of Na-excess content 被引量:2
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作者 Thongsuk Sichumsaeng Atchara Chinnakorn +3 位作者 Ornuma Kalawa Jintara Padchasri Pinit Kidkhunthod Santi Maensiri 《International Journal of Minerals,Metallurgy and Materials》 SCIE EI CAS CSCD 2023年第10期1887-1896,共10页
The effect of Na-excess content in the precursor on the structural and electrochemical performances of sodium nickel manganese oxide(NNMO)prepared by sol-gel and electrospinning methods is investigated in this paper.X... The effect of Na-excess content in the precursor on the structural and electrochemical performances of sodium nickel manganese oxide(NNMO)prepared by sol-gel and electrospinning methods is investigated in this paper.X-ray diffraction results of the prepared NNMO without adding Na-excess content indicate sodium loss,while the mixed phase of P2/O′3-type layered NNMO presented after adding Na-excess content.Compared with the sol-gel method,the secondary phase of NiO is more suppressed by using the electrospinning method,which is further confirmed by field emission scanning electron microscope images.N_(2) adsorption-desorption isotherms show no remarkably difference in specific surface areas between different preparation methods and Na-excess contents.The analysis of X-ray absorption near edge structure indicates that the oxidation states of Ni and Mn are+2 and+4,respectively.For the electrochemical properties,superior electrochemical performance is observed in the NNMO electrode with a low Na-excess content of 5wt%.The highest specific capacitance is 36.07 F·g^(-1)at0.1 A·g^(-1)in the NNMO electrode prepared by using the sol-gel method.By contrast,the NNMO electrode prepared using the electrospinning method with decreased Na-excess content shows excellent cycling stability of 100%after charge-discharge measurements for 300 cycles.Therefore,controlling the Na excess in the precursor together with the preparation method is important for improving the electrochemical performance of Na-based electrode materials in supercapacitors. 展开更多
关键词 sodium nickel manganese oxide mixed P2/O′3-type Na-excess content sol-gel method electrospinning method electrochemical properties
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Synthesis of phosphonated graphene oxide by electrochemical exfoliation to enhance the performance and durability of high-temperature proton exchange membrane fuel cells
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作者 Jianuo Chen Zunmin Guo +3 位作者 Maria Perez-Page Yifeng Jia Ziyu Zhao Stuart M.Holmes 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第1期448-458,I0011,共12页
The doping of functionalized graphene oxide(GO)in the membranes becomes a promising method for improving the performance of high-temperature proton exchange membrane fuel cells(HT-PEMFC).Phosphonated graphene oxide(PG... The doping of functionalized graphene oxide(GO)in the membranes becomes a promising method for improving the performance of high-temperature proton exchange membrane fuel cells(HT-PEMFC).Phosphonated graphene oxide(PGO)with a P/O ratio of 8.5%was quickly synthesised by one-step electrochemical exfoliation based on a three-dimensiaonal(3D)printed reactor and natural graphite flakes.Compared with the GO prepared by the two-step electrochemical exfoliation method,the PGO synthesized by the one-step electrochemical exfoliation can better improve the performance of the membrane-electrode-assembly(MEA)based on the polybenzimidazole(PBI)membrane in the HTPEMFC.The doping of 1.5 wt%GO synthesised by electrochemical exfoliation with the 2-step method or reactor method in PBI increased the peak power density by 17.4%or 35.4%compared to MEA based on pure PBI membrane at 150℃,respectively.In addition,the doping of PGO in PBI improves its durability under accelerated stress test(AST). 展开更多
关键词 electrochemical exfoliation Phosphonated graphene oxide High-temperature fuel cells
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Facet-dependent Thermal and Electrochemical Degradation of Lithium-rich Layered Oxides
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作者 Guohua Li Zhimin Ren +12 位作者 Haoxiang Zhuo Changhong Wang Biwei Xiao Jianwen Liang Ruizhi Yu Ting Lin Alin Li Tianwei Yu Wei Huang Anbang Zhang Qinghua Zhang Jiantao Wang Xueliang Sun 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2023年第6期345-355,共11页
Lithium-rich layered oxides(LLOs)are promising candidate cathode materials for safe and inexpensive high-energy-density Li-ion batteries.However,oxygen dimers are formed from the cathode material through oxygen redox ... Lithium-rich layered oxides(LLOs)are promising candidate cathode materials for safe and inexpensive high-energy-density Li-ion batteries.However,oxygen dimers are formed from the cathode material through oxygen redox activity,which can result in morphological changes and structural transitions that cause performance deterioration and safety concerns.Herein,a flake-like LLO is prepared and aberration-corrected scanning transmission electron microscopy(STEM),in situ high-temperature X-ray diffraction(HT-XRD),and soft X-ray absorption spectrum(sXAS)are used to explore its crystal facet degradation behavior in terms of both thermal and electrochemical processes.Void-induced degradation behavior of LLO in different facet reveals significant anisotropy at high voltage.Particle degradation originates from side facets,such as the(010)facet,while the close(003)facet is stable.These results are further understood through ab initio molecular dynamics calculations,which show that oxygen atoms are lost from the{010}facets.Therefore,the facet degradation process is that oxygen molecular formed in the interlayer and accumulated in the ab plane during heating,which result in crevice-voids in the ab plane facets.The study reveals important aspects of the mechanism responsible for oxygen-anionic activity-based degradation of LLO cathode materials used in lithium-ion batteries.In particular,this study provides insight that enables precise and efficient measures to be taken to improve the thermal and electrochemical stability of an LLO. 展开更多
关键词 electrochemical degradation facet degradation lithium-rich layered oxides thermal degradation
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Colour and organic removal of biologically treated coffee curing wastewater by electrochemical oxidation method 被引量:7
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作者 Rajesh S. Bejankiwar K.S. Lokesh T.P. Halappa Gowda 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2003年第3期323-327,共5页
The treatment of biologically treated wastewater of coffee-curing industry by the electrochemical oxidation using steel anode was investigated. Bench-scale experiments were conducted for activated sludge process on ra... The treatment of biologically treated wastewater of coffee-curing industry by the electrochemical oxidation using steel anode was investigated. Bench-scale experiments were conducted for activated sludge process on raw wastewater and the treated effluents were further treated by electrochemical oxidation method for its colour and organic content removal. The efficiency of the process was determined in terms of removal percentage of COD, BOD and colour during the course of reaction. Several operating parameters like time, pH and current density were examined to ascertain their effects on the treatment efficiency. Steel anode was found to be effective for the COD and colour removal with anode efficiency of 0.118 kgCOD\5h -1\5A -1\5m -2 and energy consumption 20.61 kWh\5kg -1 of COD at pH 9. The decrease in pH from 9 to 3 found to increase the anode efficiency from 0.118 kgCOD\5h -1\5A -1\5m -2 to 0.144 kWh\5kg -1 of COD while decrease the energy consumption from 20.61 kWh\5kg -1 of COD to 12.86 kWh\5kg -1 of COD. The pH of 5 was considered an ideal from the present treatment process as it avoids the addition of chemicals for neutralization of treated effluents and also economical with respect to energy consumption. An empirical relation developed for relationship between applied current density and COD removal efficiency showed strong predictive capability with coefficient of determination of 96.5%. 展开更多
关键词 electrochemical oxidation coffee-curing wastewater steel anode COD colour removal
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Indirect Electrochemical Oxidation of 4-Amino-dimethyl-aniline Hydrochloride 被引量:4
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作者 ZHANG Qiang KANG Bo +1 位作者 XU Hong LIN Hai-bo 《Chemical Research in Chinese Universities》 SCIE CAS CSCD 2006年第3期360-363,共4页
The indirect dectrechemical oxidation of 4-amino-dimethyl-aniline hydrochloride containing wastewater generated from vanillin production is presented. Experiments were conducted at a constant current density of 30 rnA... The indirect dectrechemical oxidation of 4-amino-dimethyl-aniline hydrochloride containing wastewater generated from vanillin production is presented. Experiments were conducted at a constant current density of 30 rnA/cm^2 via a Ti/Bu-Ti-Sn ternary oxide coated anode and an undivided reactor. During the various stages of the electrolysis, parameters such as the values of chemical oxygen demand(COD) and total organic carbon(TOC) were determined in order to evaluate the feasibility of the electrochemical treatment. The energy consumption and the current efficiency during the electrolysis were calculated. The present study proves the effectiveness of the electrochemical treatment for wastewater resulted from vanillin production. 展开更多
关键词 electrochemical oxidation 4-Amino-dimethyl-aniline Wastewater treatment VANILLIN
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