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Journal of Energy Chemistry 2020年第10期29卷 166-173页

作者： Shen Zhang Xing Zhang Xuerong Shi Feng Zhou Ruihu Wang Xiaoju Li Fujian Key Laboratory of Polymer Materials College of Chemistry and Materials ScienceFujian Normal UniversityFuzhou 350007FujianChina State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002FujianChina School of Material Engineering Shanghai University of Engineering Science333 Longteng RoadSongjiang DistrictShanghai 201620China

Developing active and durable electrocatalysts for overall water splitting is desirable but challenging to realize sustainable hydrogen ***,we report a facile and general method to prepare ultrafine nickel(Ni)-iridium(Ir)alloy nanoparticles/graphene hybrids for overall water *** optimized hybrid with 4.9 wt%Ir exhibits much higher catalytic activity and durability than commercial 20 wt%Ir/C for both oxygen evolution reaction(OER)and hydrogen evolution reaction(HER).Theoretical simulations reveal that the incorporation of Ir in metallic Ni lattice regulates hydrogen adsorption free energy to the optimum level,thus improving HER activity,while in situ generated amorphous Ir-Ni hydr(oxy)oxides around metallic Ni-Ir core have been demonstrated to be the active species under OER conditions,which switches OER rate-determining step to energy-favorable *** overall water splitting electrolyzer assembled by the optimized electrocatalyst shows a low cell voltage of only 1.52 V and excellent stability to deliver a current density of 10 m A *** work provides a powerful strategy toward general synthesis of ultrafine alloy nanoparticles for high-performance overall water splitting.

关键词： Alloy nanoparticles Iridium Electrocatalysts Water splitting mass activity

Atomically Adjustable Rhodium Catalyst Synthesis with Outstanding mass activity via Surface-Li mi ted Cation Exchange

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Energy & Environmental Materials 2024年第2期7卷 83-92页

作者： Hak Hyeon Lee Dong Su Kim Swagotom Sarker Ji Hoon Choi Ho Seong Lee Hyung Koun Cho Department of Advanced Materials Science&Engineering Sungkyunkwan University2066Seobu-roJangan-guSuwon-siGyeonggi-doSeoul 16419Korea Department of Advanced Materials Science&Engineering Kyungpook National University80Daehak-roBuk-guDaegu 41566Korea

Rh has been widely studied as a catalyst for the promising hydrazine oxidation reaction that can replace oxygen evolution reactions for boosting hydrogen production from hydrazine-containing *** Rh being expensive,only a few studies have examined its electrocatalytic mass ***,surface-limited cation exchange and electrochemical activation processes are designed to remarkably enhance the mass activity of *** atoms were readily replaced at the Ni sites on the surface of NiOOH electrodes by cation exchange,and the resulting RhOOH compounds were activated by the electrochemical reduction *** cation exchange-derived Rh catalysts exhibited particle sizes not exceeding 2 nm without agglomeration,indicating a decrease in the number of inactive inner Rh ***,an improved mass activity of 30 A mg_(Rh)^(-1)was achieved at 0.4 V versus reversible hydrogen ***,the two-electrode system employing the same CE-derived Rh electrodes achieved overall hydrazine splitting over 36 h at a stable low *** proposed surface-limited CE process is an effective method for reducing inactive atoms of expensive noble metal catalysts.

关键词： cation exchange synthesis electrochemical metallization hydrazine oxidation reaction mass activity rhodium catalyst

Increased utilization and mass activity of PtRu on reduced graphene oxide by heat treatment of its aerogel followed by composite with nanomaterials

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Carbon Resources Conversion 2023年第3期6卷 205-214页

作者： Kenta Dejima Hirokazu Ishitobi He Gao Mai Saito Nobuyoshi Nakagawa Graduate School of Science and Technology Gunma University1-5-1Tenjin-choKiryuGunma 376-8515Japan Division of Environmental Engineering Science Gunma University1-5-1Tenjin-choKiryuGunma 376-8515Japan Faculty of Science and Technology Gunma University1-5-1Tenjin-choKiryuGunma 376-8515Japan

The method to increase PtRu utilization and its catalytic activity of PtRu nanoparticles supported on reduced graphene oxide(RGO)by avoiding its restacking was proposed with the aim of developing an active catalyst for a direct methanol fuel *** heat treatment at 200◦C of the GO aerogel(GOA)prepared by freeze drying of GO ice was introduced to weaken the attractive force of the hydrogen bonding between the GO sheets followed by the composite with the nanoparticles,i.e.,ketjenblack(KB),TiO_(2)and Ti_(4)O_(7),at different weight *** catalyst supported on the heat-treated GOA(RGOA),PtRu/RGOA,improved the PtRu utilization to some extent and also increased the ECSA and mass activity compared to that of PtRu/*** had fewer oxygen functional groups,especially the epoxy *** to the treatment and composite,the PtRu utilization was increased from 66.5%for PtRu/RGO to 128.6%for PtRu/RGOA+Ti_(4)O_(7)(4:1)and the mass activity was improved from 50.7 A/g-PtRu for PtRu/RGO to 130.5 A/g-PtRu for PtRu/RGOA+Ti_(4)O_(7)(1:1).The Ti_(4)O_(7)nanoparticles showed the best catalytic performance for the composite suggesting that the strong interaction between Ti_(4)O_(7)and the Pt nanoparticles was effective due to its high electronic conductivity.

关键词： Reduced graphene oxide Restacking Catalyst utilization mass activity Composite catalyst Methanol oxidation Ti4O7

Synergy effects on Sn-Cu alloy catalyst for efficient CO2 electroreduction to formate with high mass activity

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Science Bulletin 2020年第9期65卷 711-719,M0003页

作者： Ke Ye Ang Cao Jiaqi Shao Gang Wang Rui Si Na Ta Jianping Xiao Guoxiong Wang State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Key Laboratory of Superlight Materials and Surface Technology of Ministry of Education College of Materials Science and Chemical EngineeringHarbin Engineering UniversityHarbin 150001China Shanghai Synchrotron Radiation Facility Zhangjiang LaboratoryShanghai 201204China

To acquire the synergy effects between Sn and Cu for the jointly high Faradaic efficiency and current density,we develop a novel strategy to design the Sn-Cu alloy catalyst via a decorated co-electrodeposition method for CO2 electroreduction to *** Sn-Cu alloy shows high formate Faradaic efficiency of 82.3%±2.1% and total C1 products Faradaic efficiency of 90.0%±2.7% at^-1.14 V *** hydrogen electrode(RHE).The current density and mass activity of formate reach as high as(79.0±0.4)mA cm^-2 and(1490.6±7.5)m A mg^-1 at^-1.14 V *** calculations suggest that Sn-Cu alloy can obtain high Faradaic efficiency for CO2 electroreduction by suppressing the competitive hydrogen evolution reaction and that the formate formation follows the path of CO2→HCOO*→*** stepped(211)surface of Sn-Cu alloy is beneficial towards selective formate production.

关键词： Electrochemical carbon dioxide reduction reaction Synergy effects Sn-Cu alloy mass activity Formate

Boron-doped amorphous iridium oxide with ultrahigh mass activity for acidic oxygen evolution reaction

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Science China Materials 2021年第12期64卷 2958-2966页

作者： Zifang Cheng Yecan Pi Qi Shao Xiaoqing Huang State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China College of Chemistry Chemical Engineering and Materials ScienceSoochow UniversitySoochow 215123China

Oxygen evolution reaction(OER), as the primary anodic reaction, plays a critical role in many electrochemical energy conversion processes. As the state-of-the-art OER catalysts, iridium-based materials are largely hindered from practical applications mainly due to the extreme scarcity of iridium. Here we demonstrate the successful fabrication of boron-doped amorphous iridium oxide(IrO_(x)-B) via a facile boric acid-assisted method, which realizes an ultrahigh OER mass activity of 2779 A g^(-1)Irat 300 mV overpotential, representing one of the best acidic OER catalysts reported so *** is found that boric acid can not only facilitate the exposure of Ir, but also dope the amorphous IrOxwith a form of metaborate, which could further modify the electronic and local ligand structure of Ir for the improved intrinsic activity. Interestingly, the reported strategy is universal that can be applied to improve other metal oxide OER catalysts, highlighting a versatile strategy for creating high-performance electrocatalysts with ultrahigh mass activity for OER and beyond.

关键词： amorphous boron iridium oxide oxygen evolution reaction mass activity

Fishbone-like platinum-nickel nanowires as an efficient electrocatalyst for methanol oxidation

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Nano Research 2020年第1期13卷 67-71页

作者： Jinquan Chang Luting Song Yuanqing Xu Yanhong Ma Cheng Liang Wenyu Jiang Yong Zhang CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing100190China University of Chinese Academy of Sciences Beijing100049China

Platinum(Pt)-based electrocatalyst with low Pt content and high electrocatalytic performance is highly desired in fuel cell ***,we demonstrated that platinum-nickel(Pt-Ni)nanowires with an average composition of PtNi3 and a fishbone structure can be readily synthesized and used as an efficient electrocatalyst toward methanol oxidation reaction(MOR).The PtNi3 fishbone-like nanowires(PtNi3-FBNWs)present features such as richer Pt on the surface than in the bulk,high-index facets on the rough surface,and polyhedral facets at the ends of side *** compositional and structural features could be determinative to the enhanced performance in the electrocatalysis of *** with commercial 20%Pt/carbon black(Pt/C),the specific activity and mass activity of the PtNi3-FBNWs are enhanced by approximately 4.76 and 3.02 times,*** stability of electrocatalysis is significantly improved as *** comprehensive enhancement indicates that the PtNi3-FBNWs would be a promising candidate toward MOR in fuel cells.

关键词： Pt-Ni nanowires(NWs) electrocatalysis specific activity mass activity methanol oxidation reaction(MOR)

硼掺杂无定形氧化铱增强酸性析氧反应质量活性（英文）

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Science China Materials 2021年

作者：成子方皮业灿邵琪黄小青 StateKeyLaboratoryofPhysicalChemistryofSolidSurfaces CollegeofChemistryandChemicalEngineeringXiamenUniversity CollegeofChemistry ChemicalEngineeringandMaterialsScienceSoochowUniversity

析氧反应（OER）作为一种主要的阳极反应,在许多电化学能量转换过程中起到了重要的作用.尽管铱（Ir）基材料是目前最先进的OER催化剂,其稀缺性很大程度上限制了该类材料的实际应用.在此,我们利用简便的硼酸辅助法成功制备了硼掺杂的无... 详细信息

析氧反应（OER）作为一种主要的阳极反应,在许多电化学能量转换过程中起到了重要的作用.尽管铱（Ir）基材料是目前最先进的OER催化剂,其稀缺性很大程度上限制了该类材料的实际应用.在此,我们利用简便的硼酸辅助法成功制备了硼掺杂的无定形氧化铱（IrOx-B）.该催化剂在300 mV过电位处展现出2779 A g-1的超高OER质量活性,是已报道的最佳酸性OER催化剂之一.我们发现硼酸不仅可以促进Ir位点的暴露,还能够以偏硼酸根的形式掺杂进入无定形IrOx中,并进一步优化Ir的电子与配位结构,进而实现本征活性的提升.有趣的是,这种方法具有一定的普适性,能够提升其他金属氧化物催化剂的OER催化活性.这为制备高质量活性的OER电催化剂提供了一种通用的策略.

关键词： amorphous boron iridium oxide oxygen evolution reaction mass activity

Pyrolysis of Iron(Ⅲ) porphyrin coated Pt/C toward oxygen reduction reaction in acidic medium

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Progress in Natural Science:Materials International 2020年第6期30卷 832-838页

作者： Yang Lv Huiyuan Liu Jiaqi Qin Rui Gao Yunlong Zhang Yan Xie Jia Li Yujiang Song State Key Laboratory of Fine Chemicals School of Chemical Engineering Dalian University of Technology Department of Mechanical and Mechatronics Engineering University of Waterloo Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of Sciences College of Engineering and Applied Sciences Nanjing University

Design and synthesis of highly active and durable electrocatalysts toward oxygen reduction reaction(ORR) is of particular importance for proton exchange membrane fuel cells(PEMFCs), yet remains a grand challenge. Herein, we report the deposition of iron(III) porphyrin(Fe P) on house-made Pt/C by rotary evaporation of the mixture of Fe P and house-made Pt/C dispersed in chloroform, followed by pyrolysis at 650 °C in argon atmosphere. This approach led to the synthesis of new non-precious metal electrocatalyst(NPME)-Pt/C composites(Pt/C–Fe P) with an average nanoparticle diameter of 3.1 ± 1.5 nm without aggregation. According to X-ray photoelectron spectroscopy(XPS), the binding energy of Pt 4 f7/2became larger due to the presence of pyrolyzed Fe P. In addition, the electrochemically active surface area(ECSA) of Pt/C–Fe P-650 is 65 m2/g less than that of house-made Pt/C(80.2 m2/g). This implies that the pyrolyzed Fe P may have partially covered the surface of Pt nanoparticles and thus lowering the ECSA. Interestingly, the mass activity(MA) of Pt/C–Fe P turns out to be 349.0 m A/mgPt@0.9 V vs. RHE, which is 2.6 times and 1.5 times of house-made Pt/C and commercial Pt/C, respectively. It is speculated that the electronic interaction and possible synergy between Pt and pyrolyzed Fe P as NPME might have contributed to the ORR activity improvement despite of partial loss of ECSA. During accelerated durability tests(ADTs), the MA of Pt/C–Fe P-650 degrades 64.3% inferior to commercial Pt/C(52.2%). The main reason likely arises from the degradation of pyrolyzed Fe P, which is a bottleneck problem confronting NPMEs.

关键词： Proton exchange membrane fuel cells Oxygen reduction reaction Electrocatalysts mass activity Durability