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构筑富含阳离子缺陷的贫P-Ni_(2)P和富P-CoP_(3)异质结用于增强尿素/肼电催化氧化反应
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作者 谭雯娟 叶勇 +7 位作者 孙秀娟 刘备 周佳佳 廖海龙 吴秀琳 丁锐 刘恩辉 高平 《物理化学学报》 SCIE CAS CSCD 北大核心 2024年第6期63-66,共4页
废水中存在的肼和尿素会对环境造成严重污染。利用电化学氧化技术处理含肼和尿素的废水,既可以有效处理废水,实现氮循环,又能将肼和尿素作为新型燃料,有助于新能源的发展。然而,目前实现肼氧化(HzOR)和尿素氧化(UOR)的电化学技术仍存在... 废水中存在的肼和尿素会对环境造成严重污染。利用电化学氧化技术处理含肼和尿素的废水,既可以有效处理废水,实现氮循环,又能将肼和尿素作为新型燃料,有助于新能源的发展。然而,目前实现肼氧化(HzOR)和尿素氧化(UOR)的电化学技术仍存在挑战。因此,开发低成本、高效且稳定性好的电催化剂是实现这一技术的先决条件。在本文中,我们采用水热-碱刻蚀-磷化的三步方法,制备了一种富含阳离子缺陷的双金属磷化物Ni_(2)P/CoP_(3)催化剂(简称Ni_(2)P/CoP_(3)-Zn^(vac)),并将其应用于肼氧化和尿素氧化。该催化剂由贫磷的Ni_(2)P和富磷的CoP_(3)两种不同性质的磷化物组成。CoP_(3)中富集的磷含有大量的负电荷,有利于吸附带正电荷的中间物种;而Ni_(2)P中磷含量较少,金属含量高,具有良好的导电性,可以确保快速的反应动力学。通过物理表征和电化学测试,证实了Ni_(2)P/CoP_(3)的成功合成和其独特的电子结构。电子顺磁测试(EPR)证明了阳离子空位的存在,大量的阳离子空位缺陷有助于增加活性位点的数量,从而提升催化性能。因此,该催化剂在肼氧化和尿素氧化方面表现出色。仅需-47 mV(HzOR)和1.311 V(UOR)的电位即可产生10 mA·cm^(-2)的电流密度。Tafel斜率分别为54.3 mV·dec^(-1)(HzOR)和37.24 mV·dec^(-1)(UOR)。Ni_(2)P/CoP_(3)-Zn^(vac)在HzOR和UOR方面的性能远优于单独的Ni_(2)P和CoP_(3),也优于未经碱刻蚀的镍钴磷化物。基于以上的测试结果,我们将Ni_(2)P/CoP_(3)-Zn^(vac)催化剂应用于直接肼燃料电池(DHzFC)和直接尿素-双氧水燃料电池(DUHPFC)的阳极,测试表明DHzFC和DUHPFC的最大功率密度分别为229.01和16.22mW·cm^(-2)。更为重要的是,DHzFC和DUHPFC能够稳定工作24 h,性能几乎不衰退。此外,Ni_(2)P/CoP_(3)-Zn^(vac)材料还可应用于自制的锌-肼燃料电池,并展示出良好的实际应用潜力。综上所述,本研究通过一系列方法制备了Ni_(2)P/CoP_(3)-Zn^(vac)催化剂,该催化剂在肼氧化和尿素氧化方面具有优异性能。这项工作为设计高效且稳定性好的肼氧化和尿素氧化电催化剂提供了新的思路。 展开更多
关键词 Ni_(2)P/CoP_(3)异质结 阳离子空位缺陷 碱刻蚀 肼氧化 尿素氧化
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Enhancing layered perovskite ferrites with ultra-high-density nanoparticles via cobalt doping for ceramic fuel cell anode
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作者 Shuo Zhai Rubao Zhao +9 位作者 hailong liao Ling Fu Senran Hao Junyu Cai Yifan Wu Jian Wang Yunhong Jiang Jie Xiao Tao Liu Heping Xie 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第9期39-48,共10页
Nanoparticles anchored on the perovskite surface have gained considerable attention for their wide-ranging applications in heterogeneous catalysis and energy conversion due to their robust and integrated structural co... Nanoparticles anchored on the perovskite surface have gained considerable attention for their wide-ranging applications in heterogeneous catalysis and energy conversion due to their robust and integrated structural configuration.Herein,we employ controlled Co doping to effectively enhance the nanoparticle exsolution process in layered perovskite ferrites materials.CoFe alloy nanoparticles with ultra-high-density are exsolved on the(PrBa)_(0.95)(Fe_(0.8)Co_(0.1)Nb_(0.1))2O_(5+δ)(PBFCN_(0.1))surface under reducing atmosphere,providing significant amounts of reaction sites and good durability for hydrocarbon catalysis.Under a reducing atmosphere,cobalt facilitates the reduction of iron cations within PBFCN_(0.1),leading to the formation of CoFe alloy nanoparticles.This formation is accompanied by a cation exchange process,wherein,with the increase in temperature,partial cobalt ions are substituted by iron.Meanwhile,Co doping significantly enhance the electrical conductivity due to the stronger covalency of the Cosingle bondO bond compared with Fesingle bondO bond.A single cell with the configuration of PBFCN_(0.1)-Sm_(0.2)Ce_(0.8)O_(1.9)(SDC)|SDC|Ba_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3−δ)(BSCF)-SDC achieves an extremely low polarization resistance of 0.0163Ωcm^(2)and a high peak power density of 740 mW cm^(−2)at 800℃.The cell also shows stable operation for 120 h in H_(2)with a constant current density of 285 mA cm^(−2).Furthermore,employing wet C_(2)H_(6)as fuel,the cell demonstrates remarkable performance,achieving peak power densities of 455 mW cm^(−2)at 800℃and 320 mW cm^(−2)at 750℃,marking improvements of 36%and 70%over the cell with(PrBa)_(0.95)(Fe_(0.9)Nb_(0.1))_(2)O_(5+δ)(PBFN)-SDC at these respective temperatures.This discovery emphasizes how temperature influences alloy nanoparticles exsolution within doped layered perovskite ferrites materials,paving the way for the development of high-performance ceramic fuel cell anodes. 展开更多
关键词 Solid oxide fuel cell ANODE Ethane fuel NANOPARTICLE EXSOLUTION Layered perovskite Ferrites
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Interfacial characteristics and mechanical properties of additive manufacturing martensite stainless steel on the Cu-Cr alloy substrate by directed energy deposition 被引量:2
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作者 Wenqi Zhang hailong liao +5 位作者 Zhiheng Hu Shasha Zhang Baijin Chen Huanqing Yang Yun Wang Haihong Zhu 《Journal of Materials Science & Technology》 SCIE EI CAS CSCD 2021年第31期121-132,共12页
Copper/steel is a typical bimetal functional material,combining the excellent electrical and thermal conductivity of copper alloy and the high strength and hardness of stainless steel.There has been recent interest in... Copper/steel is a typical bimetal functional material,combining the excellent electrical and thermal conductivity of copper alloy and the high strength and hardness of stainless steel.There has been recent interest in manufacturing copper/steel bimetal by directed energy deposition(DED)due to its layer-bylayer method.However,cracks tend to form on the copper/steel interface because of the great difference in thermal expansion coefficient and crystal structure between copper and steel.In this work,interfacial characteristics and mechanical properties of the copper/steel bimetal were studied from one layer to multilayers.The laser power has a great influence on the Cu element distribution of the molten pool,affecting the crack formation dramatically on the solidification stage.Cracks tend to form along columnar grain boundaries because of the Cu-rich liquid films and spherical particles in the cracks.Crack-free and good metallurgical bonding copper/steel interface is formed at a scanning velocity of 800 mm/min and the laser power of 3000 W.The ultimate tensile strength(UTS)and the break elongation(EL)of the vertically combined crack-free copper/steel bimetal are 238.2±4.4 MPa and 20.6±0.7%,respectively.The fracture occurs on the copper side instead of the copper/steel interface,indicating that the bonding strength is higher than that of the Cu-Cr alloy.The UTS of the horizontally combined crack-free copper/steel bimetal is 746.7±22.6 MPa,which is 200%higher than that of the Cu-Cr alloy substrate.The microhardness is 398.6±5.4 HV at the steel side and is 235.3±64.1 HV at the interface,which is400%higher than that of the Cu-Cr alloy substrate.This paper advances the understanding of the interfacial characteristics of heterogeneous materials and provides guidance and reference for the fabrication of multi-material components by DED. 展开更多
关键词 Directed energy deposition Additive manufacturing BIMETAL Interfacial characteristics CRACK
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