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A robust carbon tolerant anode for solid oxide fuel cells

Science China Materials 2015年第3期58卷 204-212页

作者：凌意瀚王振斌汪志全彭冉冉林彬于伟利 tayirjan t.isimjan 陆亚林 CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and EngineeringUniversity of Science and Technology of China Synergetic Innovation Center of Quantum Information & Quantum Physics University of Science and Technology of China Division of Physical Sciences and Engineering King Abdullah University of Scienceand Technology National Laboratory for Physical Sciences at the Microscale University of Science and Technology of China National Synchrotron Radiation Laboratory University of Science and Technology of China

Solid oxide fuel cells(SOFCs) have been attracting remarkable attention as one of the most promising green energy conversion devices in the recent ***,a high susceptibility of commonly used Ni-based anodes to carbon coking is a major challenge to the successful commercialization of *** this study,a robust anode with Ni/tiO 2-δ nano-network interfaces is reported,for low-cost SOFCs working at intermediate *** anode demonstrates an acceptable power density,and good stability with humidified(3% H2O) methane.X-ray diffraction(XRD) Rietveld refinement,X-ray photoelectron spectroscopy(XPS),electron paramagnetic resonance(EPR),and high resolution transmission electron microscopy(HRtEM) images reveal that the Ni/ti O2-δ network-composite anode forms from the in-situ reductive decomposition of Nit iO *** Ni/tiO 2-δ interfaces that facilitate the water adsorption and the water-mediated carbon-removing reactions form during this decomposition *** functional theory calculations predict that at the Ni/tiO 2-δ interfaces,the dissociated OH from H2O(adsorbed on tiO 2-δ) reacts with C(locating on Ni) to produce CO and H species,which are then electrochemically oxidized(combined with O2-) to CO2 and H2 O at the triple-phase boundaries of the anode.

关键词：固体氧化物燃料电池 Ni ti SDC 阳极

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Valence electronic engineering of superhydrophilic Dy-evoked Ni-MOF outperforming RuO_(2) for highly efficient electrocatalytic oxygen evolution

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Journal of Energy Chemistry 2024年第3期90卷 244-252,I0007页

作者： Zhiyang Huang Miao Liao Shifan Zhang Lixia Wang Mingcheng Gao Zuyang Luo tayirjan taylor isimjan Bao Wang Xiulin Yang Guangxi Key Laboratory of Low Carbon Energy Materials School of Chemistry and Pharmaceutical SciencesGuangxi Normal UniversityGulin 541004GuangxiChina State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Saudi Arabia Basic Industries Corporation(SABIC)at King Abdullah University of Science and technology(KAUSt) Thuwal 23955-6900Saudi Arabia

tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) ***,we introduce a novel strategy of dysprosium(Dy) doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of *** method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation *** and density functional theory(DFt) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and *** resulting benefits include a reduced work function and a closer proximity of the d-band center to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing ***,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics,Ex-situ and in-situ analysis results manifest Dy_(2)O_(3)/NiOOH as the actual active ***,Dy@Ni-MOF shows impressive OER performance,significantly surpassing ***,the overall water splitting device with Dy@NiMOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm^(-2) and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.

关键词： Dy@Ni-MOF Dy incorporation Electronic interaction Superhydrophilicity Oxygen evolution reaction

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Revealing interfacial charge redistribution of homologous Ru-RuS_(2) heterostructure toward robust hydrogen oxidation reaction

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Journal of Energy Chemistry 2024年第7期94卷 332-339页

作者： Yi Liu Lianrui Cheng Shuqing Zhou Yuting Yang Chenggong Niu tayirjan taylor isimjan Bao Wang Xiulin Yang Guangxi Key Laboratory of Low Carbon Energy Materials School of Chemistry and Pharmaceutical SciencesGuangxi Normal UniversityGuilin 541004GuangxiChina State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Saudi Arabia Basic Industries Corporation(SABIC)at King Abdullah University of Science and technology(KAUSt) Thuwal 23955-6900Saudi Arabia

Precisely tailoring the surface electronic structures of electrocatalysts for optimal hydrogen binding energy and hydroxide binding energy is vital to improve the sluggish kinetics of hydrogen oxidation reac-tion(HOR).Herein,we employ a partial desulfurization strategy to construct a homologous Ru-RuS_(2) heterostructure anchored on hollow mesoporous carbon nanospheres(Ru-RuS_(2)@C).the disparate work functions of the heterostructure contribute to the spontaneous formation of a unique built-in electric field,accelerating charge transfer and boosting conductivity of ***,Ru-RuS_(2)@C exhibits robust HOR electrocatalytic activity,achieving an exchange current density and mass activity as high as 3.56 mA cm^(-2) and 2.13 mAμg_(Ru)^(-1),*** those of state-of-the-art Pt/C and most contemporary Ru-based HOR ***,Ru-RuS_(2)@C can tolerate 1000 ppm of cO that lacks in Pt/*** analysis reveals that the directional electron transfer across Ru-RuS_(2) heterointerface induces local charge redistribution in interfacial region,which optimizes and balances the adsorption energies of H and OH species,as well as lowers the energy barrier for water formation,thereby promoting theHoR performance.

关键词： Heterostructure Hollow spherical structure Hydrogen oxidation reaction Charge redistribution Density functional calculation

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Phytic acid-derivative Co_(2)B-CoPO_x coralloidal structure with delicate boron vacancy for enhanced hydrogen generation from sodium borohydride

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Chinese Chemical Letters 2024年第4期35卷 525-531页

作者： Luyan Shi Ke Zhu Yuting Yang Qinrui Liang Qimin Peng Shuqing Zhou tayirjan taylor isimjan Xiulin Yang Guangxi Key Laboratory of Low Carbon Energy Materials School of Chemistry and Pharmaceutical SciencesGuangxi Normal UniversityGuilin 541004China Saudi Arabia Basic Industries Corporation(SABIC)at King Abdullah University of Science and technology(KAUSt) Thuwal 23955-6900Saudi Arabia

Application of transition metal boride(tMB) catalysts towards hydrolysis of NaBH_(4) holds great significance to help relieve the energy crisis. Herein, we present a facile and versatile metal-organic framework(MOF) assisted strategy to prepare Co_(2)B-CoPO_x with massive boron vacancies by introducing phytic acid(PA) cross-linked Co complexes that are acquired from reaction of PA and ZIF-67 into cobalt boride. the PA etching effectively breaks down the structure of ZIF-67 to create more vacancies, favoring the maximal exposure of active sites and elevation of catalytic activity. Experimental results demonstrate a drastic electronic interaction between Co and the dopant phosphorous(P), thereby the robustly electronegative P induces electron redistribution around the metal species, which facilitates the dissociation of B-H bond and the adsorption of H_(2)O molecules. the vacancy-rich Co_(2)B-CoPO_x catalyst exhibits scalable performance, characterized by a high hydrogen generation rate(HGR) of 7716.7 m L min^(-1)g^(-1) and a low activation energy(Ea) of 44.9 k J/mol, rivaling state-of-the-art catalysts. this work provides valuable insights for the development of advanced catalysts through P doping and boron vacancy engineering and the design of efficient and sustainable energy conversion systems.

关键词： Co_(2)B-CoPO_x catalyst P doping Boron vacancy NaBH_(4) hydrolysis Hydrogen generation

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构筑富含磷空位缺陷的磷化钯催化剂实现高效和抗CO毒化的碱性氢氧化反应

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Chinese Journal of Catalysis 2024年第1期56卷 176-187页

作者：杨玉婷石路岩梁沁睿刘奕董家新 tayirjan taylor isimjan 王宝杨秀林广西师范大学化学与药学学院广西低碳能源材料重点实验室中国广西桂林541004 中山大学环境科学与工程学院中国广东广州510275 中国科学院过程工程研究所生化工程国家重点实验室中国北京100190 阿卜杜拉国王科技大学的沙特阿拉伯基础工业公司图瓦勒沙特阿拉伯

碱性阴离子交换膜燃料电池(AEMFCs)可以直接将氢的化学能转化为电能,被认为是新兴绿色氢经济的基石技术.但其阳极氢氧化反应(HOR)动力学缓慢,严重依赖于Pt基催化剂.由于Pt基催化剂极易被CO毒化、动力学过程复杂以及价格昂贵,极大限制了... 详细信息

碱性阴离子交换膜燃料电池(AEMFCs)可以直接将氢的化学能转化为电能,被认为是新兴绿色氢经济的基石技术.但其阳极氢氧化反应(HOR)动力学缓慢,严重依赖于Pt基催化剂.由于Pt基催化剂极易被CO毒化、动力学过程复杂以及价格昂贵,极大限制了其商业化应用.因此,亟需开发高效、稳定和抗CO毒化能力强的新型HOR催化剂.Pd具有与Pt相似的氢键结合能,并且比Pt储量丰富,有望成为实现HOR的候选催化剂.然而,Pd的本征催化活性和Pt相比仍有很大差距.近年来,磷化钯因具有功能多样性和高催化活性被广泛关注.此外,缺陷工程可以有效调控催化剂的表面结构,改善中间体的吸附强度,提高催化剂的催化活性.因此,构建富含缺陷的磷化钯催化剂有望提高其HOR的性能.然而,该方向研究较少,反应机理尚不清楚.因此,阐明空位缺陷对于提高磷化钯催化剂HOR性能的作用机制,对促进AEMFCs电催化反应具有重要意义.本文通过溶胶-凝胶法以及低温磷化策略合成了一种碗状半球结构的富含磷空位Pd3P@C(V_(p)-Pd_(3)P@C)催化剂,并用于碱性HOR.在磷化过程中,通过调整Pd前驱体和磷源比例以及煅烧温度,在碳碗状半球载体上合成具有不同晶相组成(Pd/Pd_(3)P@C,Pd_(3.20)P_(12)@C,Pd_(3)P@C,和Pd_(5)P_(2)@C)的Pd_(x)P_(y)@C催化剂.扫描电镜和透射电镜证实了催化剂为碗状半球形貌.利用电子顺磁共振波谱研究了Pd_(x)P_(y)@C催化剂的磷空位浓度,结果表明,Pd/P比例为1:3时,在350℃下煅烧得到的Vp-Pd_(3)P@C具有最高的磷空位浓度.X射线光电子能谱证实了磷空位促进了d-p轨道杂化,增强了Pd和磷之间的电子相互作用.电化学测试结果表明,Vp-Pd_(3)P@C具有最高的HOR性能,Vp-Pd_(3)P@C在50 mV的质量活性为1.66 mAμg_(Pd)^(–1),交换电流密度为3.2 mA cm^(–2),优于Pd3P(0.45 mAμg_(Pd)^(-1),1.78 mA cm^(–2))和商业Pt/C(0.3 mAμg_(Pd)^(-1),2.29 mA cm^(–2)).同时,该催化剂在50 mV的电位下能稳定运行20 h.此外,即使在CO浓度高达1000 ppm时,Vp-Pd_(3)P@C催化剂仍表现出较好的HOR活性.紫外光电子能谱证实了Vp-Pd_(3)P@C中的Pd原子呈现缺电子状态,这不利于Pd 4d轨道对CO 2π^(*)轨道的电子反馈,降低了Pd和CO的键合强度,进而减弱了Pd对CO分子的吸附,从而增强了其抗CO中毒的能力.密度泛函理论计算结果表明,相较于磷空位浓度较少的Pd_(3)P@C催化剂,富含磷空位缺陷的Vp-Pd_(3)P@C催化剂能够优化和平衡反应中间体(Hads和OHads)的吸附强度,使速率决定步骤从H_(2)O^(*)的解吸转换到H_(2)O的形成,促进了Volmer反应(Hads+OHads→H_(2)O+2^(*)sites)的进行,进而提升了催化活性.系统实验和表征结果表明,Vp-Pd_(3)P@C较好的HOR性能可归因于以下3个因素:(1)空心碗状结构大大地增加了固-液-气三相接触点,加速了HOR的传质过程;(2)磷空位产生的局部反应活性和有利的电子结构优化了Hads和OHads的吸附强度,极大地促进了Volmer步骤;(3)丰富的磷空位打破了原有的周期性晶体结构,形成了新的电子结构,有效地抑制了电子从Pd 4d轨道到CO 2π^(*)轨道的反馈,提高了Vp-Pd_(3)P@C对CO的耐受能力.综上,本文通过缺陷工程策略调控了Vp-Pd_(3)P@C中活性位点与HOR关键中间体的相互作用,明确了空位缺陷浓度与HOR活性之间的构效关系.并从碱性HOR反应机理,CO分子与金属催化剂的轨道相互作用以及结构设计三个方面总结了高效和稳定的HOR催化剂的设计原则.目前,由于界面环境的复杂性和缺乏原位技术,催化剂表面上痕量中间体的光谱信息难以获得,未来可在开发原位技术监测HOR过程中间体和催化剂的组分变化方面做出更多的努力,以促进AEMFCs的商业化应用.

关键词：氢氧化反应 CO耐受性磷空位 V_(p)-Pd_(3)P@C 碗状半球

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Interface engineering of porous Fe^(2)P-WO_(2.92) catalyst with oxygen vacancies for highly active and stable large-current oxygen evolution and overall water splitting

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Journal of Energy Chemistry 2022年第2期31卷 574-582页

作者： Qimin Peng Qiuting He Yan Hu tayirjan taylor isimjan Ruobing Hou Xiulin Yang Guangxi Key Laboratory of Low Carbon Energy Materials School of Chemistry and Pharmaceutical SciencesGuangxi Normal UniversityGuilin 541004GuangxiChina Saudi Arabia Basic Industries Corporation(SABIC)at King Abdullah University of Science and technology(KAUSt) Thuwal 23955-6900Saudi Arabia

Constructing a low cost,and high-efficiency oxygen evolution reaction(OER)electrocatalyst is of great significance for improving the performance of alkaline electrolyzer,which is still suffering from highenergy ***,we created a porous iron phosphide and tungsten oxide self-supporting electrocatalyst with oxygen-containing vacancies on foam nickel(Fe_(2)P-WO_(2.92)/NF)through a facile insitu growth,etching and phosphating *** sequence-controllable strategy will not only generate oxygen vacancies and improve the charge transfer between Fe_(2)P and WO_(2.92) components,but also improve the catalyst porosity and expose more active *** studies illustrate that the Fe_(2)P-WO_(2.92)/NF catalyst presents good OER activity with a low overpotential of 267 mV at 100 mA cm^(-2),a small tafel slope of 46.3 mV dec^(-1),high electrical conductivity,and reliable stability at high current density(100 mA cm^(-2) for over 60 h in 1.0 M KOH solution).Most significantly,the operating cell voltage of Fe_(2)P-WO_(2.92)/NF‖Pt/C is as low as 1.90 V at 400 mA cm^(-2) in alkaline condition,which is one of the lowest reported in the *** electrocatalytic mechanism shows that the oxygen vacancies and the synergy between Fe_(2)P and WO_(2.92) can adjust the electronic structure and provide more reaction sites,thereby synergistically increasing OER *** work provides a feasible strategy to fabricate high-efficiency and stable non-noble metal OER electrocatalysts on the engineering interface.

关键词： Fe^(2)P-WO_(2.92) Interface engineering Oxygen vacancy Oxygen evolution Overall water splitting

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Delicate surface vacancies engineering of Ru doped MOF-derived Ni-NiO@C hollow microsphere superstructure to achieve outstanding hydrogen oxidation performance

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Journal of Energy Chemistry 2022年第9期31卷 395-404,I0011页

作者： Yuting Yang Yi Huang Shuqing Zhou Yi Liu Luyan Shi tayirjan taylor isimjan Xiulin Yang Guangxi Key Laboratory of Low Carbon Energy Materials School of Chemistry and Pharmaceutical SciencesGuangxi Normal UniversityGuilin 541004GuangxiChina Saudi Arabia Basic Industries Corporation(SABIC)at King Abdullah University of Science and technology(KAUSt) Thuwal 23955-6900Saudi Arabia

Surface vacancy defects,as the bridge between theoretical structural study and the design of heterogenous catalysts,have captured much *** work develops a metal-organic framework-engaged replacement-pyrolysis approach to obtain highly dispersed Ru nanoparticles immobilized on the vacancy-rich Ni-NiO@C hollow microsphere(Ru/Ni-NiO@C).Fine annealing at 400°C introduces nickel and oxygen vacancies on Ru/Ni-NiO@C surface,resulting in an improved electrical conductivity and rapid mass-charge transfer ***/Ni-NiO@C with a hollow micro/nanostructure and interconnected meso-porosity favors the maximal exposure of abundant active sites and elevation of hydrogen oxidation reaction(HOR)*** results and density functional theory(DFt)calculations reveal that an electronic effect between Ru and Ni-NiO@C,in conjunction with nickel/oxygen vacancies in the NiO species could synergistically optimize hydrogen binding energy(HBE)and hydroxide binding energy(OHBE).the HBE and OHBE optimizations thus created confer Ru/Ni-NiO@C with a mass activity over 7.75 times higher than commercial Pt/*** work may provide a constructive route to make a breakthrough in elevating the hydrogen electrocatalytic performance.

关键词： Ru/Ni-NiO@C Vacancy defects Electrocatalysis Metal-organic framework Hydrogen oxidation

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Electron-transfer enhanced MoO2-Ni heterostructures as a highly efficient pH-universal catalyst for hydrogen evolution

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Science China Chemistry 2020年第6期63卷 841-849页

作者： Benzhi Wang Hexiu Huang Meilin Huang Puxuan Yan tayirjan taylor isimjan Xiulin Yang Guangxi Key Laboratory of Low Carbon Energy Materials School of Chemistry and Pharmaceutical SciencesGuangxi Normal UniversityGuilin 541004China Saudi Arabia Basic Industries Corporation(SABIC)at King Abdullah University of Science and technology(KAUSt) Thuwal 23955-6900Saudi Arabia

Hydrogen is one of the most promising energy carriers to replace fossil fuels and electrolyzing water to produce hydrogen is a very effective ***,designing highly active and stable non-precious metal hydrogen evolution electrocatalysts that can be used in universal pH is a huge ***,we have reported a simple strategy to develop a highly active and durable non-precious MoO2-Ni electrocatalyst for hydrogen evolution reaction(HER)in a wide pH *** MoO2-Ni catalyst exhibits a superior electrocatalytic performance with low overpotentials of 46,69,and 84 mV to reach-10 mA cm-2 in 1.0 M KOH,0.5 M H2SO4,and 1.0 M PBS electrolytes,*** the same time,the catalyst also shows outstanding stability over a wide pH *** is particularly noted that the catalytic performance of MoO2-Ni in alkaline solution is comparable to the highest performing catalysts *** outstanding HER performance is mainly attributed to the collective effect of the rational morphological design,electronic structure engineering,and strong interfacial coupling between MoO2 and Ni in *** work provides a viable method for the synthesis of inexpensive and efficient HER electrocatalysts for the use in wide pH ranges.

关键词： MoO2-Ni pH-universal electron-transfer hydrogen evolution electrolysis

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Electronically modulated d-band centers of MOF-derived carbon-supported Ru/HfO_(2) for oxygen reduction and aqueous/flexible zinc-air batteries

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Journal of Energy Chemistry 2023年第5期80卷 247-255,I0007页

作者： Chuan Hu Fengli Wei Qinrui Liang Qiming Peng Yuting Yang tayirjan taylor isimjan Xiulin Yang Guangxi Key Laboratory of Low Carbon Energy Materials School of Chemistry and Pharmaceutical SciencesGuangxi Normal UniversityGuilin 541004GuangxiChina Saudi Basic Industries Corporation(SABIC)at King Abdullah University of Science and technology(KAUSt) Thuwal 23955-6900Saudi Arabia

the construction of oxide/metal composite catalysts is a competent means of exploiting the electronic interactions between oxide/metal to enhance catalytic *** this work,we construct a novel heterogeneous composite(Ru/HfO_(2)-NC)with Ru/HfO2nanoparticles nested in nitrogen-doped porous carbon via a zeolitic imidazole frameworks-assisted(ZIF)co-precipitation and calcination *** particular,ZIF guides an in-situ construction of nested configuration and confines the scattered ***,Ru/HfO_(2)-NC exhibits unusual ORR activity,superb durability,and methanol tolerance in0.1 M KOH solution with high half-wave potential(E1/2)of 0.83 V and follows a near-4e-reaction ***,the ZAB assembled with cathodic Ru/HfO_(2)-NC outputs a power density of 157.3 m W cm^(-2),a specific capacity of 775 mA h g-1Zn,and a prolonged lifespan of 258 h at 5 mA cm^(-2).Meanwhile,the catalyst has demonstrated potential applicability in flexible *** suggested by experimental results and density functional theory(DFt)analysis,the remarkable property possibly originated from the optimization of the adsorption and desorption of reactive intermediates caused by the reconfiguration of the electronic structure between Ru and HfO_(2).

关键词： Ru/HfO_(2) Charge interaction Oxygen vacancy Oxygen reduction Zinc-air battery

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Exploring the effect of Ni/Cr contents on the sheet-like NiCr-oxide-decorated CNt composites as highly active and stable catalysts for urea electrooxidation

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Clean Energy 2020年第1期4卷 58-66页

作者： Qiuping Gan Benzhi Wang Judan Chen Jianniao tian tayirjan taylor isimjan Xiulin Yang Guangxi Key Laboratory of Low Carbon Energy Materials School of Chemistry and Pharmaceutical SciencesGuangxi Normal UniversityGuilin 541004People’s Republic of China Saudi Arabia Basic Industries Corporation(SABIC)at King Abdullah University of Science and technology(KAUSt) Thuwal 23955-6900Saudi Arabia

the developing high-efficiency urea fuel cells have an irreplaceable role in solving the increasingly severe environmental crisis and energy *** sluggish six-electron dynamic anodic oxidation reaction is the bottleneck of the rapid progress of urea fuel-cell *** tackle this challenge,we select the NiCr bimetallic system due to the unique synergic effect between the Ni and the ***,better conductivity is assured using carbon nanotubes(CNts)as the *** importantly,we use a simple hydrothermal method in catalyst preparation for easy scale-up at a low *** results show that the hybrid catalysts of NiCr_(x)-oxide-CNts with different Ni/Cr ratios show much better catalytic performance in terms of active surface area and current density as compared to that of *** optimized NiCr_(2)-oxide-CNts catalyst exhibits not only the largest electrochemically active surface area(ESA,50.7 m^(2) g^(−1))and the highest urea electrocatalytic current density(115.6 mA cm^(−2)),but also outstanding long-term *** prominent performance of the NiCr_(2)-oxide-CNts catalyst is due to the combined effect of the improved charge transfer between Ni and Cr species,the large ESA,along with an elegant balance between the oxygen-defect sites and ***,we have proposed a synergistically enhanced urea catalytic mechanism.

关键词： NiCr-oxide coupling effect urea electrooxidation electrocatalysis fuel cells

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