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Metal-organic interface engineering for boosting the electroactivity of Pt nanodendrites for hydrogen production

Journal of Energy Chemistry 2020年第12期29卷 105-112页

作者： Juan Bai Nan Jia Pujun Jin Pei Chen Jia-Xing Jiang Jing-Hui Zeng Yu Chen Key Laboratory of Macromolecular Science of Shaanxi Province Key Laboratory of Applied Surface and Colloid Chemistry(MOE)Shaanxi Key Laboratory for Advanced Energy DevicesSchool of Materials Science and EngineeringShaanxi Normal UniversityXi'an 710062ShaanxiChina

Recently, the surface chemical functionalization and morphology control of precious metal nanostructures have been recognized as two efficient strategies for improving their electroactivity and/or selectivity. In this work, 1, 10-phenanthroline monohydrate(PM) functionalized Pt nanodendrites(Pt-NDs) on carbon cloth(CC)(denoted as PM@Pt-NDs/CC) and polyethylenimine(PEI) functionalized Pt-NDs on CC(denoted as PEI@Pt-NDs/CC) are successfully achieved by immersing Pt-NDs/CC into PM and PEI aqueous solutions, respectively. PEI functionalization of Pt-NDs/CC improves its electroactivity for hydrogen evolution reaction(HER) due to local proton enrichment whereas PM functionalization of Pt-NDs/CC improves its electroactivity for formic acid oxidation reaction(FAOR) by facilitating dehydrogenation pathway. With such high activity, a two-electrode electrolyzer is assembled using PM@Pt-NDs/CC as the anodic electrocatalyst and PEI@Pt-NDs/CC as the cathodic electrocatalyst for electrochemical reforming of formic acid, which only requires 0.45 V voltage to achieve the current density of 10 mA cm^(-1) for highpurity hydrogen production, much lower than conventional water electrolysis(1.59 V). The work presents an example of interfacial engineering enhancing electrocatalytic activity and indicates that electrochemical reforming of formic acid is an energy-saving electrochemical method for high-purity hydrogen production.

关键词： Pt nanodendrites Chemical functionalization Catalytic activity Hydrogen evolution reaction formic acid oxidation reaction

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Au core-PtAu alloy shell nanowires for formic acid electrolysis

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Journal of Energy Chemistry 2022年第2期31卷 94-102页

作者： Qi Xue Xin-Yu Bai Yue Zhao Ya-Nan Li Tian-Jiao Wang Hui-Ying Sun Fu-Min Li Pei Chen Pujun Jin Shi-Bin Yin Yu Chen Key Laboratory of Macromolecular Science of Shaanxi Province Key Laboratory of Applied Surface and Colloid Chemistry(MOE)Shaanxi Key Laboratory for Advanced Energy DevicesShaanxi Engineering Lab for Advanced Energy TechnologySchool of Materials Science and EngineeringShaanxi Normal UniversityXi’an 710062ShaanxiChina MOE Key Laboratory of New Processing Technology for Non-ferrous Metals and Materials Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured MaterialsGuangxi UniversityNanning 530004GuangxiChina

Inefficient electrocatalysts and high-power consumption are two thorny problems for electrochemical hydrogen(H2)production from acidic water *** 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),*** corresponding formic acid electrolyzer realizes the electrochemical H2 production at a voltage of only 0.51 V with 10 m A cm^(-2) current *** 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 *** work provides meaningful insights into the electrochemical H_(2) production from both the construction of advanced bifunctional electrocatalysts and the replacement of OER.

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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Self-catalytic induced interstitial C-doping of Pd nanoalloys for highly selective electrocatalytic dehydrogenation of formic acid

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Journal of Energy Chemistry 2023年第4期79卷 550-558页

作者： Jun Li Liying Cai Xiaosi Liang Shuke Huang Xiaosha Wang Yongshuai Kang Yongjian Zhao Lei Zhang Chenyang Zhao College of chemistry and environmental engineering Shenzhen UniversityShenzhen 518071GuangdongChina Key laboratory of optoelectronic devices and systems of ministry of education and Guangdong province College of physics and optoelectronic engineeringShenzhen UniversityShenzhen 518067GuangdongChina College of chemistry and environmental engineering Hanshan Normal UniversityChaozhou 521041GuangdongChina

Light-metalloid-atom-doped Pd interstitial nanoalloy is promising candidate for electrocatalysis because of the favorable electronic ***,an innovative method was developed to synthesize C-doped Pd interstitial nanoalloy using palladium acetate both as metal precursor and C *** characterizations demonstrated that C atoms were successfully doped into the Pd lattice via self-catalytic decomposition of acetate *** as-synthesized C-doped Pd catalysts showed excellent activity and durable stability for formic acid *** 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,*** calculations revealed that interstitial doping with C atoms induced differentiation of Pd *** strong noncovalent interaction between the Pd sites and the key intermediates endowed Pd with high-selectivity to direct routes and enhanced CO *** work presents a sites-differentiation strategy for metallic catalysts to improve the electrocatalysis.

关键词： C-doped Palladium Interstitial nanoalloy Electrocatalysis formic acid oxidation reaction

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PdNi/N-doped graphene aerogel with over wide potential activity for formic acid electrooxidation

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Journal of Energy Chemistry 2021年第8期30卷 748-754,I0016页

作者： Yufei Bao Meng Zha Pengliang Sun Guangzhi Hu Ligang Feng School of Chemical Science and Technology and Institute for Ecological Research and Pollution Control of Plateau Lakes Yunnan UniversityKunming 650504China School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China

Anti-CO poisoning ability is significant in formic acid oxidation in the fuel cell ***,Pd Ni alloy supported on N-doped graphene aerogel(Pd Ni/GA-N)was found to have catalytic ability toward formic acid electrooxidation over a wide potential range because of the improved anti-CO poisoning *** catalyst was fabricated by simple freeze-drying of mixture solution of graphene aerogel,polyvinylpyrrolidone,Pd^(2+)and Ni^(2+)and the subsequent thermal annealing reduction approach in the N2/H2 ***-Ni alloy particles anchored over the folding N-doped graphene surface with a porous hierarchical architecture structure in the 3 D *** showed the catalytic performance of its maximum mass activity of 836 m A mg^(-1)in a broad potential range(0.2-0.6 V)for formic acid *** CO stripping experiment demonstrated its largely improved anti-CO poisoning ability with the peak potential of 0.67 V,approximately 60 and 40 m V less compared to those of Pd/GA-N and Pd/C *** high anti-CO poisoning ability and strong electronic effect resulting from the interaction between the3 D GA-N support and the Pd-Ni alloy makes it a promising catalyst for application in direct formic acid fuel cells.

关键词： Fuel cells formic acid oxidation reaction PdNi Graphene aerogel

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Interfacial engineering of holey platinum nanotubes for formic acid electrooxidation boosted water splitting

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Journal of Energy Chemistry 2023年第2期77卷 209-216,I0006页

作者： Zi-Xin Ge Yu Ding Tian-Jiao Wang Feng Shi Pu-Jun Jin Pei Chen Bin He Shi-Bin Yin Yu Chen Key Laboratory of Macromolecular Science of Shaanxi Province Key Laboratory of Applied Surface and Colloid Chemistry(Ministry of Education)Shaanxi Key Laboratory for Advanced Energy DevicesShaanxi Engineering Lab for Advanced Energy TechnologySchool of Materials Science and EngineeringShaanxi Normal UniversityXi’an 710062ShaanxiChina College of New Materials and New Energies Shenzhen Technology UniversityShenzhen 518118GuangdongChina MOE Key Laboratory of New Processing Technology for Non-ferrous Metals and Materials Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured MaterialsGuangxi UniversityNanning 530004GuangxiChina

Both structure and interface engineering are highly effective strategies for enhancing the catalytic activity and selectivity of precious metal *** 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 ***,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 ***,PA modification also elevates the catalytic activity of Pt-H-NTs for the hydrogen evolution reaction(HER)by the proton enrichment at electrolyte/electrode *** 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 *** 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.

关键词： Holey platinum nanotubes Chemical functionalization formic acid oxidation reaction Hydrogen evolution reaction Water splitting

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Porous palladium phosphide nanotubes for formic acid electrooxidation

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Carbon Energy 2022年第3期4卷 283-293页

作者： Tian-Jiao Wang Yu-Chuan Jiang Jia-Wei He Fu-Min Li Yu Ding Pei Chen Yu Chen School of Materials Science and Engineering Key Laboratory of Macromolecular Science of Shaanxi ProvinceKey Laboratory of Applied Surface and Colloid Chemistry(Ministry of Education)Shaanxi Key Laboratory for Advanced Energy DevicesShaanxi Engineering Lab for Advanced Energy TechnologyShaanxi Normal UniversityXi'anChina

The development of an efficient catalyst for formic acid electrocatalytic oxidation reaction(FAEOR)is of great significance to accelerate the commercial application of direct formic acid fuel cells(DFAFC).Herein,palladium phosphide(PdxPy)porous nanotubes(PNTs)with different phosphide content(i.e.,Pd3P and Pd5P2)are prepared by combining the self-template reduction method of dimethylglyoxime-Pd(II)complex nanorods and succedent phosphating *** the reduction process,the self-removal of the template and the continual inside-outside Ostwald ripening phenomenon are responsible for the generation of the one-dimensional hollow and porous *** the basis of the unique synthetic procedure and structural advantages,Pd3P PNTs with optimized phos phide content show outstanding electroactivity and stability for *** portantly,the strong electronic effect between Pd and P promotes the direct pathway of FAEOR and inhibits the occurrence of the formic acid decomposition reaction,which effectively enhances the FAEOR electroactivity of Pd3P *** view of the facial synthesis,excellent electroactivity,high stability,and unordinary selectivity,Pd3P PNTs have the potential to be an efficient anode electrocatalyst for DFAFC.

关键词： electronic effect formic acid oxidation reaction palladium phosphide porous nanotubes self-template method

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Segmented Au/PtCo heterojunction nanowires for efficient formic acid oxidation catalysis

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Fundamental Research 2021年第4期1卷 453-460页

作者： Yingjun Sun Bolong Huang Yingjie Li Yingnan Qin Ziqi Fu Mingzi Sun Lei Wang Shaojun Guo School of Materials Science and Engineering Peking UniversityBeijing100871China College of Chemistry and Molecular Engineering Qingdao University of Science and TechnologyQingdao 266042China Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic UniversityHung HomKowloon 999077Hong Kong SARChina BIC-ESAT College of EngineeringPeking UniversityBeijing100871China

Exploring a new strategy for the removal of adsorbed CO (CO^(*)) on a Pt surface at a low potential is the key to achieving enhanced catalysis for the formic acid oxidation reaction (FAOR);however, the development of such a strategy remains a significant challenge. Herein, we report a class of Au/PtCo heterojunction nanowires (HNWs) as efficient electrocatalysts for accelerating the FAOR. This heterojunction structure and the induced Co alloying effects can facilitate formic acid adsorption/activation on Pt with high CO tolerance, generating the FAOR pathway from dehydration to dehydrogenation. The optimized Au_(23)/Pt_(63)Co_(14) HNWs showed the highest specific and mass activities of 11.7 mA cm^(−2)Pt and 6.42 A mg^(−1)Pt reported to date, respectively, which are considerably higher than those of commercial Pt/C. DFT calculations confirmed that the electron-rich Au segment enhances the electronic activity of the PtCo NWs, which not only allows the construction of a highly efficient electron transfer channel for the FAOR but also suppresses CO formation.

关键词： formic acid oxidation reaction Pt-based catalyst Heterojunction structure Nanowires Electrocatalysis

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Electrocatalytic CO_(2)and HCOOH interconversion on Pd-based catalysts

Advanced Sensor and Energy Materials

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Advanced Sensor and Energy Materials 2022年第2期1卷 12-19页

作者： Guiru Zhang Xianxian Qin Chengwei Deng Wen-Bin Cai Kun Jiang Interdisciplinary Research Center Institute of Fuel CellsSchool of Mechanical EngineeringShanghai Jiao Tong UniversityShanghai 200240China Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Collaborative Innovation Center of Chemistry for Energy MaterialsDepartment of ChemistryFudan UniversityShanghai 200438China State Key Laboratory of Space Power-Sources Technology Shanghai Institute of Space Power SourcesShanghai 200245China

Electrochemical energy storage and conversion toward sustainable carbon neutrality cycle is of great interest in today's *** this perspective,we highlight the interconversion between carbon dioxide and formic acid by means of electrocatalytic CO_(2)reduction reaction(CO_(2)RR)and formic acid oxidation reaction(FAOR)as an effective way to achieve that *** line with the distinctive catalytic nature of Pd to reversibly drive both FAOR and CO_(2)RR,we first illustrate the intimate mechanistic relation between these two reversed reactions over Pd ***,recent advances in developing Pd-based bifunctional catalysts and relevant optimization strategies are briefly summarized,including geometric structure engineering with preferential facet exposure,construction of crystallographic ordering intermetallic,electronic structure manipulation through metal or metalloid doping to fine tune the binding strength for active and poisoning *** the end,our viewpoints on the design principles at both microscopic and macroscopic scales are offered toward an efficient CO_(2)and HCOOH interconversion loop.

关键词： Carbon dioxide reduction reaction formic acid oxidation reaction Carbon neutrality reaction mechanism Palladium catalyst

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