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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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Amine-functionalized hierarchically porous carbon supported Pd nanocatalysts for highly efficient H2 generation from formic acid with fast-diffusion channels 被引量:1
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作者 Xianzhao Shao Xinyi Miao +7 位作者 Fengwu Tian Miaomiao Bai Xiaosha Guo Wei Wang Zuoping Zhao Xiaohui Ji Miyi Li Fangan Deng 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第1期249-258,I0007,共11页
Formic acid(FA)has come to be considered a potential candidate for hydrogen storage,and the development of efficient catalysts for H2releasing is crucial for realizing the sustainable process from FA.Herein,we have de... Formic acid(FA)has come to be considered a potential candidate for hydrogen storage,and the development of efficient catalysts for H2releasing is crucial for realizing the sustainable process from FA.Herein,we have developed the ultrafine Pd nanoparticle(NPs)with amine-functionalized carbon as a support,which was found to show an excellent catalytic activity in H_(2)generation from FA dehydrogenation.The synergetic mechanism between amine-group and Pd active site was demonstrated to facilitate H2generation byβ-hydride elimination.Moreover,the texture of support for Pd NPs also plays an important role in determining the reactivity of FA,since the diffusion of gaseous products makes the kinetics of diffusion as a challenge in this high performance Pd catalysts.As a result,the as-prepared Pd/NH_(2)-TPC catalyst with the small sized Pd nanoparticles and the hierarchically porous structures shows a turnover of frequency(TOF)value of 4312 h^(-1)for the additive-free FA dehydrogenation at room temperature,which is comparable to the most promising heterogeneous catalysts.Our results demonstrated that the intrinsic catalytic activities of active site as well as the porous structure of support are both important factors in determining catalytic performances in H2generation from FA dehydrogenation,which is also helpful to develop high-activity catalysts for other advanced gas-liquid-solid reactions systems. 展开更多
关键词 Hierarchically carbon Diffusion formic acid Hydrogen production Palladium nanoparticles
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Highly dispersed 1 nm Pt Pd bimetallic clusters for formic acid electrooxidation through a CO-free mechanism 被引量:1
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作者 Zhongying Fang Ziwei Zhang +8 位作者 Shemsu Ligani Fereja Jinhan Guo Xinjie Tong Yue Zheng Rupeng Liu Xiaolong Liang Leting Zhang Zongjun Li Wei Chen 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第3期554-564,I0015,共12页
Direct formic acid fuel cell(DFAFC) is an important research project in clean energy field.However,commercialization of DFAFC is still largely limited by the available catalysts with unsatisfied activity,durability an... Direct formic acid fuel cell(DFAFC) is an important research project in clean energy field.However,commercialization of DFAFC is still largely limited by the available catalysts with unsatisfied activity,durability and cost for formic acid electrooxidation(FAEO).Using Pt-and Pd-based nanoclusters as electrocatalysts is a particularly promising strategy to solve the above problem,but two attendant problems need to be solved firstly.(Ⅰ) The controllable synthesis of practicable and stable sub-2 nm clusters remains challenging.(Ⅱ) The catalyzing mechanism of sub-2 nm metal clusters for FAEO has not yet completely understood.Herein,different from traditional solution synthesis,by designing a novel supporting material containing electron-rich and electron-deficient functional groups,size-and dispersioncontrollable synthesis of ~1 nm PtPd nanoclusters is realized by an electrochemical process.The electrocatalytic properties and reaction mechanism of the PtPd nanoclusters for the FAEO were studied by different electrochemical techniques,in-situ fourier transform infrared(FTIR) spectra and density functional theory(DFT) calculations.The tiny PtPd nanoclusters have much higher catalytic activity and durability than commercial Pt/C,Pd/C and 3.5 nm PtPd nanoparticles.The present study shows that the metalreactant interaction plays a decisive role in determining the catalytic activity and cluster-support interaction plays a decisive role in enhancing the durability of electrocatalyst.The ratio and arrangement of Pt and Pd atoms on the surface of 1 nm PtPd cluster as well as the overall valence state,d-band center and specific surface area make them exhibit different catalytic performance and reaction mechanism from nanoparticle catalysts.In addition,in situ FTIR and DFT calculations showed that on the surface of PtPd clusters,the generation of CO_(2)through trans-COOH intermediate is the most optimal reaction pathway for the FAEO. 展开更多
关键词 CLUSTER formic acid oxidation ELECTROCATALYSIS In situ FTIR Reaction mechanism
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Ti-Fe_(2)O_(3)/Ni(OH)_(x) as an efficient and durable photoanode for the photoelectrochemical catalysis of PET plastic to formic acid 被引量:1
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作者 Xin Li Jianying Wang +2 位作者 Mingze Sun Xufang Qian Yixin Zhao 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第3期487-496,I0014,共11页
Photoelectrochemical(PEC) technology provides a promising prospect for the transformation of polyethylene terephthalate(PET) plastic wastes to produce value-added chemicals.The PEC catalytic systems with high activity... Photoelectrochemical(PEC) technology provides a promising prospect for the transformation of polyethylene terephthalate(PET) plastic wastes to produce value-added chemicals.The PEC catalytic systems with high activity,selectivity and long-term durability are required for the future up-scaling industrial applications.Herein,we employed the interfacial modification strategy to develop an efficient and stable photoanode and evaluated its PEC activity for ethylene glycol(EG,derived from PET hydrolysate) oxidation to formic acid.The interfacial modification between Fe_(2)O_(3)semiconductor and Ni(OH)xcocatalyst with ultrathin TiO_(x) interlayer not only improved the photocurrent density by accelerating the kinetics of photogenerated charge carriers,but also kept the high Faradaic efficiency(over 95% in 30 h) towards the value-added formic acid product.This work proposes an effective method to promote the PEC activity and enhance the long-term stability of photoelectrodes for upcycling PET plastic wastes. 展开更多
关键词 Plastic waste formic acid Photoelectrochemical catalysis High durability Interfacial modification
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Self-catalytic induced interstitial C-doping of Pd nanoalloys for highly selective electrocatalytic dehydrogenation of formic acid
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作者 Jun Li Liying Cai +6 位作者 Xiaosi Liang Shuke Huang Xiaosha Wang Yongshuai Kang Yongjian Zhao Lei Zhang Chenyang Zhao 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第4期550-558,共9页
Light-metalloid-atom-doped Pd interstitial nanoalloy is promising candidate for electrocatalysis because of the favorable electronic effect.Herein,an innovative method was developed to synthesize C-doped Pd interstiti... Light-metalloid-atom-doped Pd interstitial nanoalloy is promising candidate for electrocatalysis because of the favorable electronic effect.Herein,an innovative method was developed to synthesize C-doped Pd interstitial nanoalloy using palladium acetate both as metal precursor and C dopant.Elaborate characterizations demonstrated that C atoms were successfully doped into the Pd lattice via self-catalytic decomposition of acetate ions.The as-synthesized C-doped Pd catalysts showed excellent activity and durable stability for formic acid electrooxidation.The mass activity and specific activity at 0.6 V of C-doped Pd were approximately 2.59 A/mg and 3.50 mA cm^(-2),i.e.,2.4 and 2.6 times of Pd,respectively.DFT calculations revealed that interstitial doping with C atoms induced differentiation of Pd sites.The strong noncovalent interaction between the Pd sites and the key intermediates endowed Pd with high-selectivity to direct routes and enhanced CO tolerance.This work presents a sites-differentiation strategy for metallic catalysts to improve the electrocatalysis. 展开更多
关键词 C-doped PALLADIUM Interstitial nanoalloy ELECTROCATALYSIS formic acid oxidation reaction
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Pt-Te alloy nanowires towards formic acid electrooxidation reaction
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作者 Bin Sun Yu-Chuan Jiang +5 位作者 Qing-Ling Hong Xue Liu Fu-Min Li Dong-Sheng Li Yun Yang Yu Chen 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第10期481-489,I0013,共10页
The high-performance anodic electrocatalysts is pivotal for realizing the commercial application of the direct formic acid fuel cells.In this work,a simple polyethyleneimine-assisted galvanic replacement reaction is a... The high-performance anodic electrocatalysts is pivotal for realizing the commercial application of the direct formic acid fuel cells.In this work,a simple polyethyleneimine-assisted galvanic replacement reaction is applied to synthesize the high-quality PtTe alloy nanowires(PtTe NW)by using Te NW as an efficient sacrificial template.The existence of Te atoms separates the continuous Pt atoms,triggering a direct reaction pathway of formic acid electrooxidation reaction(FAEOR)at PtTe NW.The one-dimensional architecture and highly active sites have enabled PtTe NW to reveal outstanding electrocatalytic activity towards FAEOR with the mass/specific activities of 1091.25 mA mg^(-1)/45.34 A m^(-2)at 0.643 V potential,which are 44.72/23.16 and 20.26/11.75 times bigger than those of the commercial Pt and Pd nanoparticles,respectively.Density functional theory calculations reveal that Te atoms optimize the electronic structure of Pt atoms,which decreases the adsorption capacity of CO intermediate and simultaneously improves the durability of PtTe NW towards FAEOR.This work provides the valuable insights into the synthesis and design of efficient Pt-based alloy FAEOR electrocatalysts. 展开更多
关键词 formic acid electrooxidation PtTe alloy nanowires Galvanic replacement reaction Reaction pathway Fuel cells
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Interfacial engineering of holey platinum nanotubes for formic acid electrooxidation boosted water splitting
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作者 Zi-Xin Ge Yu Ding +6 位作者 Tian-Jiao Wang Feng Shi Pu-Jun Jin Pei Chen Bin He Shi-Bin Yin Yu Chen 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第2期209-216,I0006,共9页
Both structure and interface engineering are highly effective strategies for enhancing the catalytic activity and selectivity of precious metal nanostructures.In this work,we develop a facile pyrolysis strategy to syn... Both structure and interface engineering are highly effective strategies for enhancing the catalytic activity and selectivity of precious metal nanostructures.In this work,we develop a facile pyrolysis strategy to synthesize the high-quality holey platinum nanotubes(Pt-H-NTs)using nanorods-like Pt^(Ⅱ)-phenanthroline(PT)coordination compound as self-template and self-reduction precursor.Then,an up-bottom strategy is used to further synthesize polyallylamine(PA)modified Pt-H-NTs(Pt-HNTs@PA).PA modification sharply promotes the catalytic activity of Pt-H-NTs for the formic acid electrooxidation reaction(FAEOR)by the direct reaction pathway.Meanwhile,PA modification also elevates the catalytic activity of Pt-H-NTs for the hydrogen evolution reaction(HER)by the proton enrichment at electrolyte/electrode interface.Benefiting from the high catalytic activity of Pt-H-NTs@PA for both FAEOR and HER,a two-electrode FAEOR boosted water electrolysis system is fabricated by using Pt-H-NTs@PA as bifunctio nal electrocatalysts.Such FAEOR boosted water electrolysis system only requires the operational voltage of 0.47 V to achieve the high-purity hydrogen production,showing an energy-saving hydrogen production strategy compared to traditional water electrolysis system. 展开更多
关键词 Holey platinum nanotubes Chemical functionalization formic acid oxidation reaction Hydrogen evolution reaction Water splitting
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High-Con cent rat ion Electrosynthesis of Formic Acid/Formate from CO_(2):Reactor and Electrode Design Strategies
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作者 Yizhu Kuang Hesamoddin Rabiee +4 位作者 Lei Ge Thomas E.Rufford Zhiguo Yuan John Bell Hao Wang 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2023年第6期141-157,共17页
The electrochemical CO_(2)reduction reaction(CO_(2)RR),driven by renewable energy,provides a potential carbon-neutral avenue to convert CO_(2)into valuable fuels and feedstocks.Conversion of CO_(2)into formic acid/for... The electrochemical CO_(2)reduction reaction(CO_(2)RR),driven by renewable energy,provides a potential carbon-neutral avenue to convert CO_(2)into valuable fuels and feedstocks.Conversion of CO_(2)into formic acid/formate is considered one of the economical and feasible methods,owing to their high energy densities,and ease of distribution and storage.The separation of formic acid/formate from the reaction mixtures accounts for the majority of the overall CO_(2)RR process cost,while the increment of product concentration can lead to the reduction of separation cost,remarkably.In this paper,we give an overview of recent strategies for highly concentrated formic acid/formate products in CO_(2)RR.CO_(2)RR is a complex process with several different products,as it has different intermediates and reaction pathways.Therefore,this review focuses on recent study strategies that can enhance targeted formic acid/formate yield,such as the all-solid-state reactor design to deliver a high concentration of products during the reduction of CO_(2)in the electrolyzer.Firstly,some novel electrolyzers are introduced as an engineering strategy to improve the concentration of the formic acid/formate and reduce the cost of downstream separations.Also,the design of planar and gas diffusion electrodes(GDEs)with the potential to deliver high-concentration formic acid/formate in CO_(2)RR is summarized.Finally,the existing technological challenges are highlighted,and further research recommendations to achieve high-concentration products in CO_(2)RR.This review can provide some inspiration for future research to further improve the product concentration and economic benefits of CO_(2)RR. 展开更多
关键词 electrochemical CO_(2)reduction reaction electrode design formic acid/formate high-concentration reactor design
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Photoelectrocatalytic reduction of CO_2 into formic acid using WO_(3-x)/TiO_2 film as novel photoanode 被引量:2
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作者 杨亚辉 解人瑞 +3 位作者 黎航 刘灿军 刘文华 占发琦 《Transactions of Nonferrous Metals Society of China》 SCIE EI CAS CSCD 2016年第9期2390-2396,共7页
A novel WO3-x/TiO2 film as photoanode was synthesized for photoelectrocatalytic(PEC) reduction of CO2 into formic acid(HCOOH). The films prepared by doctor blade method were characterized with X-ray diffractometer... A novel WO3-x/TiO2 film as photoanode was synthesized for photoelectrocatalytic(PEC) reduction of CO2 into formic acid(HCOOH). The films prepared by doctor blade method were characterized with X-ray diffractometer(XRD), scanning electron microscope(SEM) and transmission electron microscope(TEM). The existence of oxygen vacancies in the WO3-x was confirmed with an X-ray photoelectron spectroscopy(XPS), and the accurate oxygen index was determined by a modified potentiometric titrimetry method. After 3h of photoelectrocatalytic reduction, the formic acid yield of the WO3-x/TiO2 film is 872 nmol/cm^2, which is 1.83 times that of the WO3/TiO2 film. The results of PEC performance demonstrate that the introduction of WO3-x nanoparticles can improve the charge transfer performance so as to enhance the performance of PEC reduction of CO2 into formic acid. 展开更多
关键词 photoelectrocatalytic reduction CO2 formic acid WO3-x TiO2 film photoanode
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A Revisit to the Role of Bridge-adsorbed Formate in the Electrocatalytic Oxidation of Formic Acid at Pt Electrodes 被引量:1
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作者 徐杰 梅东 +3 位作者 袁道福 张尊彪 刘少雄 陈艳霞 《Chinese Journal of Chemical Physics》 SCIE CAS CSCD 2013年第3期321-328,I0004,共9页
The mechanism and kinetics of electrocatalytic oxidation of formic acid at Pt electrodes is discussed in detail based on previous electrochemical in-situ ATR-FTIRS data [Langmuir 22, 10399 (2006)and Angewa. Chem. In... The mechanism and kinetics of electrocatalytic oxidation of formic acid at Pt electrodes is discussed in detail based on previous electrochemical in-situ ATR-FTIRS data [Langmuir 22, 10399 (2006)and Angewa. Chem. Int. Ed. 50, 1159 (2011)]. A kinetic model with formic acid adsorption (and probably the simultaneous C-H bond activation) as the rate determining step, which contributes to the majority of reaction current for formic acid oxi- dation, was proposed for the direct pathway. The model simulates well the IR spectroscopic results obtained under conditions where the poisoning effect of carbon monoxide (CO) is negligible and formic acid concentration is below 0.1 mol/L. The kinetic simulation predicts that in the direct pathway formic acid oxidation probably only needs one Pt atom as active site, formate is the site blocking species instead of being the active intermediate. We review in detail the conclusion that formate pathway (with either 1st or 2nd order reaction kinetics) is the direct pathway, possible origins for the discrepancies are pointed out. 展开更多
关键词 formic acid oxidation Mechanism ELECTROCATALYSIS Formate pathway Directpathway
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Pt-Containing Ag_2S-Noble Metal Nanocomposites as Highly Active Electrocatalysts for the Oxidation of Formic Acid 被引量:1
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作者 Hui Liu Yan Feng +1 位作者 Hongbin Cao Jun Yang 《Nano-Micro Letters》 SCIE EI CAS 2014年第3期252-257,共6页
Nanocomposites with synergistic effect are of great interest for their enhanced properties in a given application. Herein, we reported the high catalytic activity of Pt-containing Ag2S-noble metal nanocomposites in fo... Nanocomposites with synergistic effect are of great interest for their enhanced properties in a given application. Herein, we reported the high catalytic activity of Pt-containing Ag2S-noble metal nanocomposites in formic acid oxidation, which is a key reaction in direct formic acid fuel cell. The electrochemical measurements including voltammograms and chronoamperograms are used to characterize the catalytic property of Pt-containing nanocomposites for the oxidation of formic acid. In view of the limited literatures on using nanocomposites consisting of semiconductor and noble metals for catalyzing the reactions of polymer electrolyte membrane-based fuel cells, this study provides a helpful exploration for expanding the application of semiconductor-noble metal nanocomposites. 展开更多
关键词 NANOCOMPOSITES Synergistic effect formic acid oxidation Direct formic acid fuel cell
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Unveiling the decomposition mechanism of formic acid on Pd/WC(0001) surface by using density function theory 被引量:1
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作者 Jinhua Zhang Yuanbin She 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2020年第3期415-425,共11页
In pursuit of low-cost direct formic acid fuel cells,tungsten carbide(WC)supported Pd catalyst is considered as an ideal candidate for efficient decomposition of formic acid due to low Pd utilization and excellent per... In pursuit of low-cost direct formic acid fuel cells,tungsten carbide(WC)supported Pd catalyst is considered as an ideal candidate for efficient decomposition of formic acid due to low Pd utilization and excellent performance.Herein,different adsorption configurations and active sites of the intermediates,involved in the HCOOH decomposition,on WC(0001)-supported Pd monolayer(Pd/WC(0001))surface investigated by using density functional theory.The results reveal that trans-HCOOH,HCOO,cis-COOH,trans-COOH,HCO,CO,H2 O,OH and H exhibit chemisorption on Pd/WC(0001)surface,whereas cis-HCOOH and CO2 exhibit weak interactions with Pd/WC(0001)surface.In addition,the minimum energy pathways of HCOOH decomposition are analyzed to generate CO and CO2 due to the fracture of C–H,H–O and C–O bonds.The adsorbed HCOOH,HCOO,mH COO,cis-COOH and trans-COOH configurations exhibit dissociation rather than desorption.CO formation occurs through the decomposition of cis-COOH,trans-COOH and HCO,whereas the CO2 formation happens due to the decomposition of HCOO.It is found that the most favorable pathway for HCOOH decomposition on Pd/WC(0001)surface is HCOOH→HCOO→CO2,where the formation of CO2 from HCOO dehydrogenation determines the reaction rate.Overall,CO2 is the most dominant product of HCOOH decomposition on Pd/WC(0001)surface.The presence of WC,as monolayer Pd carrier,does not alter the catalytic behavior of Pd and significantly reduces the Pd utilization. 展开更多
关键词 Density functional theory formic acid Direct formic acid fuel cells WC(0001)-supported Pd monolayer Decomposition mechanism
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Hydrothermal synthesis of titanium-supported nanoporous palladium-copper electrocatalysts for formic acid oxidation and oxygen reduction reaction
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作者 易清风 肖兴中 刘云清 《Transactions of Nonferrous Metals Society of China》 SCIE EI CAS CSCD 2013年第4期1184-1190,共7页
Nanoporous Pd and binary Pd-Cu particles were prepared by a hydrothermal method using ethylene glycol as a reduction agent and they were directly immobilized on Ti substrates named as Ti-supported Pd-based catalysts. ... Nanoporous Pd and binary Pd-Cu particles were prepared by a hydrothermal method using ethylene glycol as a reduction agent and they were directly immobilized on Ti substrates named as Ti-supported Pd-based catalysts. Their electrocatalytic activity for formic acid oxidation and oxygen reduction reaction (ORR) in alkaline media was examined by voltammetric techniques. Among the as-prepared catalysts, nanoPdslCu19/Ti catalyst presents the highest current density of 39.8 mA/cm2 at -0.5 V or 66.4 mA/cm2 at -0.3 V for formic acid oxidation. The onset potential of ORR on the nanoPdslCU19/Ti catalyst presents an about 70 mV positive shift compared to that on the nanoPd/Ti, and the current density of ORR at -0.3 V is 2.12 mA/cm2, which is 3.7 times larger than that on the nanoPd/Ti. 展开更多
关键词 Pd electrode Pd-Cu electrode formic acid oxidation oxygen reduction reaction NANOPARTICLE ELECTROCATALYSIS
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Pd micro-nanoparticles electrodeposited on graphene/polyimide membrane for electrocatalytic oxidation of formic acid 被引量:3
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作者 张焱 王琴 +2 位作者 叶为春 李佳佳 王春明 《Transactions of Nonferrous Metals Society of China》 SCIE EI CAS CSCD 2015年第9期2986-2993,共8页
A novel Pd electrocatalyst with flowerlike micro-nanostructures was synthesized by electrochemical deposition on a flexible graphene/polyimide(Gr/PI) composite membrane and characterized by scanning electron microsc... A novel Pd electrocatalyst with flowerlike micro-nanostructures was synthesized by electrochemical deposition on a flexible graphene/polyimide(Gr/PI) composite membrane and characterized by scanning electron microscopy(SEM),X-ray diffraction(XRD).The Pd micro-nanoparticles were prepared on a COOH-CNTs/PI membrane as a comparative sample.The XRD and SEM investigations for Pd electrodeposition demonstrate that the particle size of Gr/PI composite membrane is smaller than that of COOH-CNTs/PI membrane,while the uniform and dense distribution of Pd micro-nanoparticles on the Gr/PI composite membrane is greater than that on the COOH-CNTs/PI membrane.The electrocatalytic properties of Pd/Gr/PI and Pd/COOH-CNTs/PI catalysts for the oxidation of formic acid were investigated by cyclic voltammetry(CV) and chronoamperometry(CA).It is found that the electrocatalytic activity and stability of Pd/Gr/PI are superior to those of Pd/COOH-CNTs/PI catalyst.This is because smaller metal particles and higher dense distribution desirably provide abundant catalytic sites and mean higher catalytic activity.Therefore,the Pd/Gr/PI catalyst has better catalytic performance for formic acid oxidation than the Pd/COOH-CNTs/PI catalyst. 展开更多
关键词 Pd micro-nanoparticles graphene/polyimide membrane carboxyl carbon nanotubes/polyimide membrane electro catalytic oxidation formic acid electrochemical deposition
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Role of Bridge-bonded Formate in Formic Acid Dehydration to CO at Pt Electrode: Electrochemial in-situ Infrared Spectroscopic Study 被引量:1
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作者 张尊彪 徐杰 +1 位作者 康婧 陈艳霞 《Chinese Journal of Chemical Physics》 SCIE CAS CSCD 2013年第4期471-476,J0002,共7页
Formic acid (HCOOH) decomposition at Pt film electrode has been studied by electrochem- ical in situ FTIR spectroscopy under attenuated-total-reflection configuration, in order to clarify whether bridge-bonded forma... Formic acid (HCOOH) decomposition at Pt film electrode has been studied by electrochem- ical in situ FTIR spectroscopy under attenuated-total-reflection configuration, in order to clarify whether bridge-bonded formate (HCOOD) is the reactive intermediate for COad for-mation from HCOOH molecules. When switching from HCOOH-free solution to HCOOH- containing solution at constant potential (E=0.4 V vs. RHE), we found that immediately upon solution switch COad formation rate is the highest, while surface coverage of formate is zero, then after COad formation rate decreases, while formate coverage reaches a steady state coverage quickly within ca. 1 s. Potential step experiment from E=0.75 V to 0.35 V, reveals that formate band intensity drops immediately right after the potential step, while the COad signal develops slowly with time. Both facts indicate that formate is not the reactive intermediate for formic acid dehydration to CO. 展开更多
关键词 Mechanism for formic acid dehydration Formate intermediate CO pathway Pt electrode Infrared spectroscopic studies under attenuated total reflection configuration
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Preparation of Ultrafine and High Dispersion Pd/C Catalyst and Its Electrocatalytic Performance for Formic Acid Oxidation 被引量:8
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作者 TANG Ya-wen ZHANG Lin-lin +4 位作者 WANG Xin BAO Jian-chun ZHOU Yi-ming LU Lu-de LU Tian-hong 《Chemical Research in Chinese Universities》 SCIE CAS CSCD 2009年第2期239-242,共4页
A carbon supported Pd(Pd/C) catalyst used as the anodic catalyst in the direct formic acid fuel cells(DFAFC) was prepared via the improved complex reduction method with sodium ethylenediamine tetracetate(EDTA) a... A carbon supported Pd(Pd/C) catalyst used as the anodic catalyst in the direct formic acid fuel cells(DFAFC) was prepared via the improved complex reduction method with sodium ethylenediamine tetracetate(EDTA) as stabilizer and complexing agent. This method is very simple. The average size of the Pd particles in the Pd/C catalyst prepared with the improved complex reduction method is as small as about 2.1 nm and the Pd particles in the Pd/C catalyst possess an excellent uniformity. The Pd/C catalyst shows a high electrocatalytic activity and stability for the formic acid oxidation. 展开更多
关键词 Pd/C catalyst Complex reduction method formic acid oxidation
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MoS2/Zn3In2S6 composite photocatalysts for enhancement of visible light-driven hydrogen production from formic acid 被引量:9
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作者 Sujuan Zhang Shixiang Duan +5 位作者 Gaoli Chen Sugang Meng Xiuzhen Zheng You Fan Xianliang Fu Shifu Chen 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2021年第1期193-204,共12页
Enhancing the separation efficiency of photogenerated carriers is propitious for the promotion of photocatalytic hydrogen production from formic acid decomposition.Herein,MoS2/Zn3In2S6(MoS2/ZIS6)composite photocatalys... Enhancing the separation efficiency of photogenerated carriers is propitious for the promotion of photocatalytic hydrogen production from formic acid decomposition.Herein,MoS2/Zn3In2S6(MoS2/ZIS6)composite photocatalysts containing varying mass percentages of MoS2 were obtained by a straightforward synthetic method.The results confirmed that MoS2,as a cocatalyst,markedly promoted the photogenerated charge separation efficiency and visible light-driven hydrogen production activity of ZIS6(λ>400 nm).Specifically,the as-prepared 0.5%MoS2/ZIS6 photocatalyst exhibited the highest photocatalytic hydrogen production rate(74.25μmol·h^-1),which was approximately 4.3 times higher than that of ZIS6(17.47μmol·h^-1).The excellent performance of the 0.5%MoS2/ZIS6 photocatalyst may be due to the fact that MoS2 has a low Fermi energy level and can thus enrich photogenerated electrons from ZIS6,and furthermore reduce H+derived from formic acid,to form hydrogen.The structure and morphology of the MoS2/ZIS6 photocatalysts and the reactive species were determined by X-ray diffraction,transmission electron microscopy,and field emission scanning electron microscopy,among others;a plausible mechanistic rationale is discussed based on the results. 展开更多
关键词 Hydrogen production Zn3In2S6 formic acid MOS2 PHOTOCATALYSIS
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Rough-surfaced bimetallic copper–palladium alloy multicubes as highly bifunctional electrocatalysts for formic acid oxidation and oxygen reduction 被引量:4
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作者 Dong Chen Linlin Xu +1 位作者 Hui Liu Jun Yang 《Green Energy & Environment》 SCIE CSCD 2019年第3期254-263,共10页
Engineering the morphology of nanomaterials and modifying their electronic structure are effective ways to improve their performance in electrocatalysis. Through combining the co-reduction of Pd2+ and Cu2+ precursors ... Engineering the morphology of nanomaterials and modifying their electronic structure are effective ways to improve their performance in electrocatalysis. Through combining the co-reduction of Pd2+ and Cu2+ precursors with a digestive ripening process in oleylamine, we report the synthesis of copper-palladium(Cu-Pd) alloy multicubes with rough surfaces. Benefiting from their alloy and unique rough-surfaced structure,which provides ample edge/corner and step atoms as well as the electronic coupling between Cu and Pd leading to the lower of d-band center, the rough-surfaced Cu-Pd alloy multicubes show much better electrocatalytic performance not only for formic acid oxidation but also for oxygen reduction in comparison with those of spherical Cu-Pd alloy nanoparticles and commercial Pd/C catalyst. In contrast, we confirm that the rough-surfaced Cu-Pd alloy multicubes only exhibit very low Faradaic efficiency(34.3%) for electrocatalytic conversion of carbon dioxide(CO2) to carbon monoxide(CO) due to the presence of strong competing hydrogen evolution reaction, which results in their very poor selectivity for the reduction of CO2 to CO. The findings in this study not only offer a promising strategy to produce highly effective electrocatalysts for direct formic acid fuel cells, but also enlighten the ideas to design efficient electrocatalysts for CO2 reduction. 展开更多
关键词 Copper–palladium Multicube formic acid oxidation Oxygen REDUCTION CO2 REDUCTION
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Surface interaction between Pd and nitrogen derived from hyperbranched polyamide towards highly effective formic acid dehydrogenation 被引量:4
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作者 Yancun Yu Xian Wang +3 位作者 Changpeng Liu Fateev Vladimir Junjie Ge Wei Xing 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2020年第1期212-216,I0008,共6页
Hydrogen production from formic acid decomposition(FAD)is a promising means of hydrogen energy storage and utilization in fuel cells.Development of efficient catalysts for dehydrogenation of formic acid is a challengi... Hydrogen production from formic acid decomposition(FAD)is a promising means of hydrogen energy storage and utilization in fuel cells.Development of efficient catalysts for dehydrogenation of formic acid is a challenging topic.The surface chemical and electronic structure of the active catalysis components is important in formic acid decomposition at room-temperature.Here,the pyrdinic-nitrogen doped catalysts from hyperbranched polyamide were prepared via in situ polymerization reaction process by using activated carbon as a support.Because of the introduction of the polymer,the particles of the catalysts were stabilized,and the average particle diameter was only 1.64 nm.Under mild conditions,the catalysts activities were evaluated for FAD.The optimized Pd-N30/C catalyst exhibited high performance achieving almost full conversion,with a turnover frequency of 3481 h^-1 at 30℃. 展开更多
关键词 formic acid decomposition Hydrogen generation Hyperbranched polymer Pd catalyst
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Au core-PtAu alloy shell nanowires for formic acid electrolysis 被引量:7
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作者 Qi Xue Xin-Yu Bai +8 位作者 Yue Zhao Ya-Nan Li Tian-Jiao Wang Hui-Ying Sun Fu-Min Li Pei Chen Pujun Jin Shi-Bin Yin Yu Chen 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第2期94-102,共9页
Inefficient electrocatalysts and high-power consumption are two thorny problems for electrochemical hydrogen(H2)production from acidic water electrolysis.Herein we report the one-pot precise synthesis of ultrafine Au ... Inefficient electrocatalysts and high-power consumption are two thorny problems for electrochemical hydrogen(H2)production from acidic water electrolysis.Herein we report the one-pot precise synthesis of ultrafine Au core-Pt Au alloy shell nanowires(Au@PtxAu UFNWs).Among them,Au@Pt_(0.077) Au UFNWs exhibit the best performance for formic acid oxidation reaction(FAOR)and hydrogen evolution reaction(HER),which only require applied potentials of 0.29 V and-22.6 m V to achieve a current density of 10 m A cm^(-2),respectively.The corresponding formic acid electrolyzer realizes the electrochemical H2 production at a voltage of only 0.51 V with 10 m A cm^(-2) current density.Density functional theory(DFT)calculations reveal that the Au-riched Pt Au alloy structure can facilitates the direct oxidation pathway of FAOR and consequently elevates the FAOR activity of Au@Pt_(0.077) Au UFNWs.This work provides meaningful insights into the electrochemical H_(2) production from both the construction of advanced bifunctional electrocatalysts and the replacement of OER. 展开更多
关键词 Au core-PtAu alloy shell nanowires formic acid oxidation reaction Reaction pathway Hydrogen evolution reaction Acidic water electrolysis
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