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活性炭电催化氧化技术降解废水中氯苯机理研究 被引量:4
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作者 李国平 王彧 +2 位作者 夏明芳 王志良 杨振亚 《环境科技》 2011年第1期1-4,共4页
采用活性炭电催化氧化技术,研究氯苯降解机理。配制质量浓度100 mg/L的氯苯水溶液,在活性炭电催化反应器槽电流1.0 A,降解时间为10~120 min条件下,采用高效液相色谱仪和气-质联用仪定性分析氯苯降解产物,研究氯苯降解过程;控制降解时间... 采用活性炭电催化氧化技术,研究氯苯降解机理。配制质量浓度100 mg/L的氯苯水溶液,在活性炭电催化反应器槽电流1.0 A,降解时间为10~120 min条件下,采用高效液相色谱仪和气-质联用仪定性分析氯苯降解产物,研究氯苯降解过程;控制降解时间30min,在槽电流分别为0.5,1.0,2.0A条件下,分析水样中强氧化剂.OH含量。研究结果表明,不同的时间,废水中氯苯降解生成的中间产物不同,中间产物主要有对氯苯酚、对苯二酚、对苯醌、丁烯二酸和草酸等;氯苯废水在电催化作用下,产生具有强氧化能力的·OH,其降解过程为:·OH先攻击苯环Cl基团的对位,在亲电加成作用下生成对氯苯酚,Cl基团再被·OH取代生成对苯二酚和对苯醌,接着被氧化开环形成有机酸类物质,最终被矿化为CO_2和H_2O,但有机酸矿化的过程比较缓慢。 展开更多
关键词 氯苯 降解机理 活性催化氧化
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Pt及其修饰电极对丙三醇氧化的电催化性能研究 被引量:3
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作者 陈国良 陈声培 +3 位作者 林珩 许振芳 林洵 孙世刚 《厦门大学学报(自然科学版)》 CAS CSCD 北大核心 2002年第2期211-216,共6页
运用电化学循环伏安和石英晶体微天平研究了丙三醇在Pt电极和以Sb ,S吸附原子修饰的Pt (Pt/Sbad和Pt/Sad)电极上的吸附和氧化过程 .结果表明丙三醇的氧化与电极表面氧物种有着极其密切的关系 .Pt电极表面Sb吸附原子能在较低的电位下吸附... 运用电化学循环伏安和石英晶体微天平研究了丙三醇在Pt电极和以Sb ,S吸附原子修饰的Pt (Pt/Sbad和Pt/Sad)电极上的吸附和氧化过程 .结果表明丙三醇的氧化与电极表面氧物种有着极其密切的关系 .Pt电极表面Sb吸附原子能在较低的电位下吸附氧 ,可显著提高丙三醇电催化氧化活性 ,与Pt电极相比较 ,Sb吸附原子修饰的Pt电极使丙三醇氧化的峰电位负移了 0 .14V .相反 ,Pt电极表面S吸附原子的氧化会消耗表面氧物种 ,几乎完全抑制了丙三醇的电氧化 . 展开更多
关键词 石英晶体微天平 PT 修饰 丙三醇 吸附 氧化 电催化氧化活性 化学循环伏安法
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咪唑四氟硼酸盐离子液体中磷钼酸掺杂聚吡咯薄膜修饰电极的制备及其电催化活性
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作者 王文敏 李章林 鄢浩 《化学研究》 CAS 2013年第3期277-280,共4页
以1-丁基-3-甲基咪唑四氟硼酸盐(BMIMBF4)离子液体作为介质,利用电化学方法在铂电极表面制备了磷钼酸掺杂聚吡咯薄膜;采用扫描电子显微镜观察了所制备的薄膜的形貌,利用热重分析评价了其热稳定性,利用循环伏安法测定了其电化学活性和对... 以1-丁基-3-甲基咪唑四氟硼酸盐(BMIMBF4)离子液体作为介质,利用电化学方法在铂电极表面制备了磷钼酸掺杂聚吡咯薄膜;采用扫描电子显微镜观察了所制备的薄膜的形貌,利用热重分析评价了其热稳定性,利用循环伏安法测定了其电化学活性和对甲醇的电催化氧化活性.结果表明,与传统的硫酸溶液相比,以BMI-MBF4离子液体作为反应介质制备的修饰电极的表面形貌更均匀,电化学活性和对甲醇的电催化氧化活性更强. 展开更多
关键词 离子液体 磷钼酸掺杂 聚吡咯薄膜 修饰 制备 电催化氧化活性
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High activity of a Pt decorated Ni/C nanocatalyst for hydrogen oxidation 被引量:3
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作者 高孝麟 王昱飞 +2 位作者 谢和平 刘涛 储伟 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2017年第2期396-403,共8页
The Pt decorated Ni/C nanocatalysts were prepared for hydrogen oxidation reaction(HOR) in fuel cell.By regulating the contents of Pt and Ni in the catalyst,both the composition and the structure affected the electro... The Pt decorated Ni/C nanocatalysts were prepared for hydrogen oxidation reaction(HOR) in fuel cell.By regulating the contents of Pt and Ni in the catalyst,both the composition and the structure affected the electrochemical catalytic characteristics of the Pt-Ni/C catalysts.When the Pt mass content was 3.1% percent and that of Ni was 13.9% percent,the Pt-Ni/C-3 catalyst exhibited a larger electrochemically active surface area and a higher exchange current density toward HOR than those of pure supported platinum sample.Our study demonstrates a feasible approach for designing the more efficient catalysts with lower content of noble metal for HOR in fuel cell. 展开更多
关键词 Platinum catalyst Galvanic displacement Nickel supported on carbon Hydrogen oxidation reaction Electrochemically active surface
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Pt alloy oxygen-reduction electrocatalysts: Synthesis, structure, and property 被引量:17
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作者 Xiao Xia Wang Joshua Sokolowski +1 位作者 Hui Liu Gang Wu 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2020年第5期739-755,共17页
Proton exchange membrane fuel cells(PEMFCs) are considered a promising power source for electric vehicles and stationary residential applications. However, current PEMFCs have several problems that require solutions, ... Proton exchange membrane fuel cells(PEMFCs) are considered a promising power source for electric vehicles and stationary residential applications. However, current PEMFCs have several problems that require solutions, including high cost, insufficient power density, and limited performance durability. A kinetically sluggish oxygen reduction reaction(ORR) is primarily responsible for these issues. The development of advanced Pt-based catalysts is crucial for solving these problems if the large-scale application of PEMFCs is to be realized. In this review, we summarize the recent progress in the development of Pt M alloy(M = Fe, Co, Ni, etc.) catalysts with an emphasis on ordered Pt M intermetallic catalysts, which exhibit significantly enhanced activity and stability. In addition to exploring the intrinsic catalytic performance in traditional aqueous electrolytes via engineering nanostructures, morphologies, and crystallinity of Pt M particles, we highlight recent efforts to study catalysts under real fuel cell environments by the membrane electrode assembly(MEA). 展开更多
关键词 Proton exchange membrane fuel cell Oxygen reduction reaction Low Pt catalyst Catalytic activity Stability
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Structure-dependent electrocatalytic activity of La_(1-x)SrxMnO_3 for oxygen reduction reaction 被引量:2
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作者 Guangjin Wang Tian Xu +1 位作者 Sheng Wen Mu Pan 《Science China Chemistry》 SCIE EI CAS CSCD 2015年第5期871-878,共8页
The electrocatalytic activity toward oxygen reduction reaction is studied on the perovskite oxide La~_xbrxMnt)3, as preparea under different firing temperatures. X-ray diffraction shows that three different crystal p... The electrocatalytic activity toward oxygen reduction reaction is studied on the perovskite oxide La~_xbrxMnt)3, as preparea under different firing temperatures. X-ray diffraction shows that three different crystal phases featuring tetragonal, cubic, and orthorhombic symmetries form with increasing crystallinities. The electrocatalytic activity is characterized by cyclic voltam- metry and linear sweeping voltammetry for the three phases of La1-xSrxMnO3. We find that the tetragonal phase has the best catalytic activity among the three crystal phases, with the largest onset potential of 0.147 V. The synergistic effect between the volume per unit cell and crystallinity is indicated to account for the good catalytic activity of the tetragonal phase. 展开更多
关键词 perovskite oxide LA1-XSRXMNO3 crystal phase CRYSTALLINITY oxygen reduction reaction
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Behavior of gold-enhanced electrocatalytic performance of NiPtAu hollow nanocrystals for alkaline methanol oxidation 被引量:6
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作者 Chang Liu Zelin Chen +5 位作者 Dewei Rao Jinfeng Zhang Yunwei Liu Yanan Chen Yida Deng Wenbin Hu 《Science China Materials》 SCIE EI CSCD 2021年第3期611-620,共10页
The Pt-based catalyst tends to be poisoned by carbon monoxide(CO)-like intermediates produced in fuel cell reactions,which seriously deteriorates its catalytic performance.Herein,noble metal Au with the capacity of re... The Pt-based catalyst tends to be poisoned by carbon monoxide(CO)-like intermediates produced in fuel cell reactions,which seriously deteriorates its catalytic performance.Herein,noble metal Au with the capacity of resistance to CO-like intermediates poisoning was employed to construct multi-element Pt-based catalysts.Two trimetallic NiPtAu hollow nanocrystals(HNCs)with different surface Au contents were synthesized to explore the role of Au in electrocatalysis for alkaline methanol oxidation reaction(MOR).The trimetallic NiPtAu-SRAu HNCs catalyst with the relative rich Au content(15.17 at%)on surface exhibits a much lower CO oxidation peak potential than the other HNCs counterpart and 20 wt%Pt/C,which indicates the more exceptional CO-resisting performance.Besides,the MOR specific activity of NiPtAu-SRAu HNCs(31.52 mA cm^−2)is 7 times higher than that of 20wt%Pt/C(4.50 mA cm^−2).This enhancement in catalytic activity as well as anti-CO poisoning capability for NiPtAu-SRAu HNCs can be mainly ascribed to the weakened CO adsorption due to the exposure of Au atoms on NiPt surface evidenced by the experimental data and density functional theory calculations.This study not only investigates the role of Au in MOR catalysis but also could be helpful for designing and optimizing the electrocatalysts for high-active and robust fuel cell applications. 展开更多
关键词 trimetallic NiPtAu hollow nanocrystals methanol oxidation carbon monoxide poisoning
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Facile synthesis of Fe/Ni bimetallic oxide solid-solution nanoparticles with superior electrocatalytic activity for oxygen evolution reaction 被引量:13
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作者 Lingxiao Wang Jing Geng Wenhai Wang Chao Yuan Long Kuai Baoyou Geng 《Nano Research》 SCIE EI CAS CSCD 2015年第12期3815-3822,共8页
The sluggish oxygen evolution reaction (OER) is an important half-reaction of the electrochemical water-splitting reaction. Amorphous Fe/Ni composite oxides have high activity. In this work, we modified the aerosol ... The sluggish oxygen evolution reaction (OER) is an important half-reaction of the electrochemical water-splitting reaction. Amorphous Fe/Ni composite oxides have high activity. In this work, we modified the aerosol spray-assisted approach and obtained amorphous Fe-Ni-Ox solid-solution nanoparticles (Fe-Ni-Ox-NPs) approximately 20 nm in size by choosing iron/nickel acetylacetonates as raw materials instead of inorganic salts. The small-sized Fe-Ni-Ox-NPs were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD) analysis, energy-dispersive X-ray spectroscopy (EDX), and X-ray photoelectron spectroscopy (XPS). Furthermore, an investigation of electrochemical OER performance suggests that the small-sized Fe-Ni-Ox-NPs have higher activity than the large-sized Fe-Ni-Ox-MPs. A small overpotential of 0.315 V was demanded to obtain a working current density of 50 mA/cm2, and the Tafel slope was as low as 38 mWdec. 展开更多
关键词 Fe-Ni-Ox solid solution ELECTROCATALYSIS oxygen evolution reaction
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Maximizing the visible light photoelectrochemical activity of B/N-doped anatase TiO_2 microspheres with exposed dominant {001} facets 被引量:2
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作者 Xingxing Hong1 2 +11 位作者 Yuyang Kang1 2 Chao Zhen1 Xiangdong Kang1 Li-Chang Yin1 John TS Irvine3 Lianzhou Wang4 Gang Liu1 2 Hui-Ming Cheng1 5 6 《Science China Materials》 SCIE EI CSCD 2018年第6期831-838,共8页
Anatase TiO2 microspheres with exposed dominant {001} facets were doped with interstitial boron to have a concentration gradient with the maximum concentration at the surface. They were then further doped with substit... Anatase TiO2 microspheres with exposed dominant {001} facets were doped with interstitial boron to have a concentration gradient with the maximum concentration at the surface. They were then further doped with substitutional nitrogen by heating in an ammonia atmosphere at different temperatures from 440 to 560℃ to give surface N concentrations ranging from 7.03 to 15.47 at%. The optical absorption, atomic and electronic structures and visible-light photoelectrochemical water oxidation activity of these materials were investigated. The maximum activity of the doped TiO2 was achieved at a nitrogen doping temperature of 520℃ that gave a high absorbance over the whole visible light region but with no defect-related background absorption. 展开更多
关键词 PHOTOELECTROCHEMISTRY red TiO2 water splitting doping
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Regulating the electronic structure of NiFe layered double hydroxide/reduced graphene oxide by Mn incorporation for high-efficiency oxygen evolution reaction 被引量:6
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作者 Binbin Jiang Weng-Chon Cheong +9 位作者 Renyong Tu Kaian Sun Shoujie Liu Konglin Wu Hengshuai Shang Aijian Huang Miao Wang Lirong Zheng Xianwen Wei Chen Chen 《Science China Materials》 SCIE EI CAS CSCD 2021年第11期2729-2738,共10页
The development of highly efficient and costeffective oxygen evolution reaction(OER)electrocatalysts for renewable energy systems is vitally essential.Modulation of the electronic structure through heteroatom doping i... The development of highly efficient and costeffective oxygen evolution reaction(OER)electrocatalysts for renewable energy systems is vitally essential.Modulation of the electronic structure through heteroatom doping is considered as one of the most potential strategies to boost OER performances.Herein,a rational design of Mn-doped NiFe layered double hydroxide/reduced graphene oxide(Mn-NiFe LDH/rGO)is demonstrated by a facile hydrothermal approach,which exhibits outstanding OER activity and durability.Experimental results and density functional theory(DFT)calculations manifest that the introduction of Mn can reprogram the electronic structure of surface active sites and alter the intermediate adsorption energy,consequently reducing the potential limiting activation energy for OER.Specifically,the optimal Mn-NiFe LDH/rGO composite shows an enhanced OER performance with an ultralow overpotential of 240 mV@10 mA cm^(-2),Tafel slope of 40.0 mV dec^(-1) and excellent stability.Such superior OER activity is comparable to those of the recently reported state-of-the-art OER catalysts.This work presents an advanced strategy for designing electrocatalysts with high activity and low cost for energy conversion applications. 展开更多
关键词 MN NiFe layered double hydroxides ELECTROCATALYSTS oxygen evolution reaction DFT calculations
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Enhanced electrocatalytic oxidation of dyes in aqueous solution using cobalt phthalocyanine modified activated carbon fiber anode 被引量:2
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作者 LI Nan DONG SuSu +4 位作者 LV WangYang HUANG SanQing CHEN HaiXiang YAO YuYuan CHEN WenXing 《Science China Chemistry》 SCIE EI CAS 2013年第12期1757-1764,共8页
Cobalt tetra(2,4-dichloro-1,3,5-triazine)aminophthalocyanine (CoPc) was immobilized covalently on activated carbon fiber (ACF) felt to obtain CoPc-modified ACF (CoPc-ACF) catalyst, and an electrocatalytic oxid... Cobalt tetra(2,4-dichloro-1,3,5-triazine)aminophthalocyanine (CoPc) was immobilized covalently on activated carbon fiber (ACF) felt to obtain CoPc-modified ACF (CoPc-ACF) catalyst, and an electrocatalytic oxidation system using CoPc-ACF as the anode was constructed. The electrocatalytic oxidation of Acid Red 1 (ARI) was investigated in aqueous solution by an UV-vis spectrophotometer and UPLC. The results indicated that AR1 could be eliminated efficiently in this electrocatalytic oxidation system. In addition, the results of FTIR, TOC and GC-MS suggested that the electrocatalytic oxidation experienced the decoloration achieved by destroying the azo linkage and the further mineralization due to the cleavages of benzene ring and naphthalene ring. The intermediates were mainly small molecular compounds such as maleic acid and succinic acid, etc. Re- petitive tests showed that CoPc-ACF can maintain high electrocatalytic activity over several cycles. The further EPR spin-trap experiments indicated that the hydroxyl radicals did not dominate the reaction in this electrocatalytic system, which was com- pletely different from the traditional electro-Fenton system. Based on the non-radical reaction mechanism, the CoPc-modified ACF electrocatalyst has potential application in treating actual dyestuffs wastewaters, which are accompanied with high concentration of hydroxyl radical scavengers such as chlorine ions and additives in the textile printing and dyeing industry. 展开更多
关键词 DYES electrocatalytic oxidation activated carbon fiber cobalt phthalocyanine
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Influence of Cl substitution on the electronic structure and catalytic activity of ceria 被引量:1
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作者 Li-Li Yin Xue-Qing Gong 《Science China Chemistry》 SCIE EI CAS CSCD 2015年第4期601-606,共6页
Cl-containing cerium dioxide(Ce O2) catalysts have been found to exhibit unique catalytic activities. In the present work, using density functional theory calculations with the inclusion of on-site Coulomb correction,... Cl-containing cerium dioxide(Ce O2) catalysts have been found to exhibit unique catalytic activities. In the present work, using density functional theory calculations with the inclusion of on-site Coulomb correction, we systematically studied the effect of Cl on the physicochemical properties of Ce O2 surfaces by substituting one subsurface O with Cl. The calculated results show that substituting an O atom with a Cl atom results in structural distortion and the reduction of one surface Ce4+ cation to Ce3+. The protruding Ce3+ cation greatly improves the adsorption energy of O2 to produce an active O2- species, and maintains the catalytic oxidation cycle of CO on Ce O2(110). These results may help us obtain a better understanding of Cl-ceria interacting systems and provide some guidance for the design of effective Ce O2-based catalysts. 展开更多
关键词 cerium dioxide Cl substitution DFT+U O2 adsorption CO oxidation
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Insight on the active sites of CoNi alloy embedded in N-doped carbon nanotubes for oxygen reduction reaction 被引量:1
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作者 Ying Wang Miaomiao Tong +3 位作者 Lei Wang Xu Liu Chungui Tian Honggang Fu 《Science China Materials》 SCIE EI CAS CSCD 2021年第11期2719-2728,共10页
Transition metal alloy electrocatalysts have sparked intense interest for their use in oxygen reduction reaction(ORR).However,there is almost no corresponding research on the alloy active sites.In this study,CoNi allo... Transition metal alloy electrocatalysts have sparked intense interest for their use in oxygen reduction reaction(ORR).However,there is almost no corresponding research on the alloy active sites.In this study,CoNi alloy nanoparticles embedded in bamboo-like N-doped carbon nanotubes(CoNi-NCTs)as catalysts constructed by a facile pyrolysis of Prussian blue analogs were investigated.The density functional theory calculation reveals that the oxygen molecules are more easily adsorbed on the Ni sites in these catalysts,while the Co sites favor the formation of OOH★intermediates during ORR.In addition,the cooperation of the CoNi alloys with the N-doped carbon benefits electron transfer and promotes electrocatalytic activity.The optimized CoNi-NCT shows remarkable ORR catalytic activity with an half-wave potential(E1/2)of 0.83 V,an onset potential(Eonset)of 0.97 V,and superior durability,all of which surpass the commercial Pt/C catalysts.The assembled zinc-air battery delivers a small charge/discharge voltage gap of 0.86 V at 10 mA cm^(-2),a high-power density of 167 mW cm^(-2),and good stability(running stably over 900 cycles). 展开更多
关键词 N-doped carbon nanotube CoNi alloy active site oxygen reduction reaction Zn-air battery
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WB crystals with oxidized surface as counter electrode in dye-sensitized solar cells
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作者 Jian Pan Chao Zhen +2 位作者 Lianzhou Wang Gang Liu Hui-Ming Cheng 《Science Bulletin》 SCIE EI CAS CSCD 2017年第2期114-118,共5页
Tungsten boride(WB) crystals, whose surface tends to be oxidized when exposed to air, were demonstrated to have a comparable activity to platinum as counter electrode material in dye-sensitized solar cells. The synerg... Tungsten boride(WB) crystals, whose surface tends to be oxidized when exposed to air, were demonstrated to have a comparable activity to platinum as counter electrode material in dye-sensitized solar cells. The synergistic effect of both catalytically active surface layer WOxand electronically conductive internal WB is considered to be responsible for the high activity of the WB crystals. 展开更多
关键词 Counter electrode Tungsten boride Dye-sensitized solar cell Tungsten oxide
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Shape-controlled Pt nanocubes directly grown on carbon supports and their electrocatalytic activity toward methanol oxidation 被引量:5
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作者 Hee Jin Kim Bibi Ruqia +6 位作者 Mi Sung Kang Su Bin Lim Ran Choi Ki Min Nam Won Seok Seo Gaehang Lee Sang-Il Choi 《Science Bulletin》 SCIE EI CAS CSCD 2017年第13期943-949,共7页
Synthesis of shape-controlled Pt nanocrystals is substantial and important for enhancing chemical and electrochemical reactions.However,the removal of capping agents,shape-controlling chemicals,on Pt surfaces is essen... Synthesis of shape-controlled Pt nanocrystals is substantial and important for enhancing chemical and electrochemical reactions.However,the removal of capping agents,shape-controlling chemicals,on Pt surfaces is essential prior to conducting the catalytic reactions.Here we report a facile one-pot synthesis of Pt nanocubes directly grown on carbon supports(Pt nanocubes/C) with modulating the kinetic reaction factors for shaping the nanocrystals,but without adding any capping agents for preserving the clean Pt surfaces.Well-dispersed Pt nanocubes/C shows enhanced activity and long-term stability toward methanol oxidation reaction compared to the commercial Pt/C catalyst. 展开更多
关键词 Platinum Nanocube Shape-control Kinetic product Methanol oxidation
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