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1.
Hongyang Su Lanlan Chen Yizhen Chen Prof. Rui Si Yuting Wu Xiaonan Wu Dr. Zhigang Geng Prof. Wenhua Zhang Prof. Jie Zeng 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(46):20591-20596
Efforts have been devoted to achieving a highly efficient artificial synthesis of ammonia (NH3). Reported herein is a novel Fe-MoS2 catalyst with Fe atomically dispersed onto MoS2 nanosheets, imitating natural nitrogenase, to boost N2 electroreduction into NH3 at room temperature. The Fe-MoS2 nanosheets exhibited a faradic efficiency of 18.8 % with a yield rate of 8.63 μg mgcat.−1 h−1 for NH3 at −0.3 V versus the reversible hydrogen electrode. The mechanism study revealed that the electroreduction of N2 was promoted and the competing hydrogen evolution reaction was suppressed by decorating the edge sites of S in MoS2 with the atomically dispersed Fe, resulting in high catalytic performance for the electroreduction of N2 into NH3. This work provides new ideas for the design of catalysts for N2 electroreduction and strengthens the understanding about N2 activation over Mo-based catalysts. 相似文献
2.
Hydrogen Spillover Enhanced Hydroxyl Formation and Catalytic Activity Toward CO Oxidation at the Metal/Oxide Interface 下载免费PDF全文
Yuekang Jin Guanghui Sun Feng Xiong Liangbing Ding Prof. Dr. Weixin Huang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(11):4252-4256
H2‐promoted catalytic activity of oxide‐supported metal catalysts in low‐temperature CO oxidation is of great interest but its origin remains unknown. Employing an FeO(111)/Pt(111) inverse model catalyst, we herewith report direct experimental evidence for the spillover of H(a) adatoms on the Pt surface formed by H2 dissociation to the Pt?FeO interface to form hydroxyl groups that facilely oxidize CO(a) on the neighboring Pt surface to produce CO2. Hydroxyl groups and coadsorbed water play a crucial role in the occurrence of hydrogen spillover. These results unambiguously identify the occurrence of hydrogen spillover from the metal surface to the noble metal/metal oxide interface and the resultant enhanced catalytic activity of the metal/oxide interface in low‐temperature CO oxidation, which provides a molecular‐level understanding of both H2‐promoted catalytic activity of metal/oxide ensembles in low‐temperature CO oxidation and hydrogen spillover. 相似文献
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正Chemical reactions catalyzed by solid catalysts have recently expanded rapidly from traditional heterogeneous catalytic reactions to photocatalytic reactions and further to plasmonic-catalytic reactions,however,the fundamental understanding of the commonalities and differences among heterogeneous catalysis, 相似文献
4.
To improve the response performance of superconducting infrared detectors, we propose using a photonic antenna with a micro-detector in conjunction with a nano-structure. In this paper, we report evaluation results that show the basic characteristics of a photonic antenna in the mid-infrared region. The antenna consists of a nano-slot antenna and a thin-film load resistance placed in the center of the antenna. The antennas were designed for operation at approximately several tens of THz by using an electromagnetic simulator. Through measurements of the spectral reflectance characteristics, clear absorptions caused by the antenna properties were observed at approximately 50 THz, and high polarization dependencies were also observed. The results of the simulation qualitatively agreed with the results of the experiment. The effective area of the antenna was also evaluated and was found to be approximately 3.5 μm2 at 54 THz. 相似文献
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利用X射线衍射、N2吸附等温线、X射线光电子能谱、X射线吸收谱、H2-程序升温还原、甲基橙选择化学吸附和等电点测定等方法研究了共沉淀方法制备的一系列CexTi1-xO2复合氧化物的结构. 成功发展了甲基橙选择化学吸附和等电点方法研究CexTi1-xO2复合氧化物的最外层表面结构, 并定义了“等价CeO2表面覆盖度”来描述CexTi1-xO2复合氧化物的最外层表面结构. CexTi1-xO2复合氧化物 (x ≥ 0.7)形成立方萤石相固溶体, Ce0.3Ti0.7O2表现出纯的单斜相, 而其它复合氧化物表现出混合相. CexTi1-xO2复合氧化物最外层表面结构的演变行为不同于其体相结构.Ce0.7Ti0.3O2立方萤石相固溶体最外层表面已经部分形成了单斜相Ce0.3Ti0.7O2, 随Ce含量的降低, 单斜相Ce0.3Ti0.7O2从最外层表面向体相生长. CexTi1-xO2复合氧化物立方萤石相固溶体和单斜相Ce0.3Ti0.7O2分别在相对较低和较高的温度表现出好的还原性能. 上述结果提供了全面和深层次的CexTi1-xO2复合氧化物结构信息. 相似文献
6.
Zhaorui Li Dr. Kristin Werner Lu Chen Aiping Jia Dr. Kun Qian Dr. Jian-Qiang Zhong Dr. Rui You Dr. Lihui Wu Liyuan Zhang Dr. Haibin Pan Prof. Dr. Xin-Ping Wu Prof. Dr. Xue-Qing Gong Dr. Shamil Shaikhutdinov Prof. Weixin Huang Prof. Dr. Hans-Joachim Freund 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(16):5268-5276
The study reports the first attempt to address the interplay between surface and bulk in hydride formation in ceria (CeO2) by combining experiment, using surface sensitive and bulk sensitive spectroscopic techniques on the two sample systems, i.e., CeO2(111) thin films and CeO2 powders, and theoretical calculations of CeO2(111) surfaces with oxygen vacancies (Ov) at the surface and in the bulk. We show that, on a stoichiometric CeO2(111) surface, H2 dissociates and forms surface hydroxyls (OH). On the pre-reduced CeO2−x samples, both films and powders, hydroxyls and hydrides (Ce−H) are formed on the surface as well as in the bulk, accompanied by the Ce3+ ↔ Ce4+ redox reaction. As the Ov concentration increases, hydroxyl is destabilized and hydride becomes more stable. Surface hydroxyl is more stable than bulk hydroxyl, whereas bulk hydride is more stable than surface hydride. The surface hydride formation is the kinetically favorable process at relatively low temperatures, and the resulting surface hydride may diffuse into the bulk region and be stabilized therein. At higher temperatures, surface hydroxyls can react to produce water and create additional oxygen vacancies, increasing its concentration, which controls the H2/CeO2 interaction. The results demonstrate a large diversity of reaction pathways, which have to be taken into account for better understanding of reactivity of ceria-based catalysts in a hydrogen-rich atmosphere. 相似文献
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《Solid State Ionics》2006,177(13-14):1205-1210
A comparative investigation of the much-studied La2NiO4+δ (n = 1) phase and the higher-order Ruddlesden-Popper phases, Lan+1NinO3n+1 (n = 2 and 3), has been undertaken to determine their suitability as cathodes for intermediate-temperature solid-oxide fuel cells. As n is increased, a structural phase transition is observed from tetragonal I4/mmm in the hyperstoichiometric La2NiO4.15 (n = 1) to orthorhombic Fmmm in the oxygen-deficient phases, La3Ni2O6.95 (n = 2) and La4Ni3O9.78 (n = 3). High temperature d.c. electrical conductivity measurements reveal a dramatic increase in overall values from n = 1, 2 to 3 with metallic behavior observed for La4Ni3O9.78. Impedance spectroscopy measurements on symmetrical cells with La0.9Sr0.10Ga0.80Mg0.20O3−δ (LSGM-9182) as the electrolyte show a systematic improvement in the electrode performance from La2NiO4.15 to La4Ni3O9.78 with ∼ 1 Ω cm2 observed at 1073 K for the latter. Long-term thermal stability tests show no impurity formation when La3Ni2O6.95 and La4Ni3O9.78 are heated at 1123 K for 2 weeks in air, in contrast to previously reported data for La2NiO4.15. The relative thermal expansion coefficients of La3Ni2O6.95 and La4Ni3O9.78 were found to be similar at ∼ 13.2 × 10− 6 K− 1 from 348 K to 1173 K in air compared to 13.8 × 10− 6 K− 1 for La2NiO4.15. Taken together, these observations suggest favourable use for the n = 2 and 3 phases as cathodes in intermediate-temperature solid-oxide fuel cells when compared to the much-studied La2NiO4+δ (n = 1) phase. 相似文献
9.
FeOx Coating on Pd/C Catalyst by Atomic Layer Deposition Enhances the Catalytic Activity in Dehydrogenation of Formic Acid 下载免费PDF全文
Hydrogen generation from formic acid (FA) has received significant attention.The challenge is to obtain a highly active catalyst under mild conditions for practical applications.Here atomic layer deposition (ALD) of FeOx was performed to deposit an ultrathin oxide coating layer to a Pd/C catalyst,therein the FeOx coverage was precisely controlled by ALD cycles.Transmission electron microscopy and powder X-ray diffraction measurements suggest that the FeOx coating layer improved the thermal stability of Pd nanoparticles (NPs).X-ray photoelectron spectroscopy measurement showed that deposition of FeOx on the Pd NPs caused a positive shift of Pd3d binding energy.In the FA dehydrogenation reaction,the ultrathin FeOx layer on the Pd/C could considerably improve the catalytic activity,and Pd/C coated with 8 cycles of FeOx showed an optimized activity with turnover frequency being about 2 times higher than the uncoated one.The improved activities were in a volcanoshape as a function of the number of FeOx ALD cycles,indicating the coverage of FeOx is critical for the optimized activity.In summary,simultaneous improvements of activity and thermal stability of Pd/C catalyst by ultra-thin FeOx overlayer suggest to be an effective way to design active catalysts for the FA dehydrogenation reaction. 相似文献
10.
Chen Li Wendong Wang Congying Xu Yuanxu Liu Bo He Chusheng Chen .CAS Key Laboratory of Materials for Energy Conversion University of Science Technology of China Hefei Anhui China 《天然气化学杂志》2011,(4):345-349
The double perovskite oxides Sr2Mg1-xF exMoO6-δ were investigated as catalysts for the methane oxidation.The structural properties of catalysts were characterized in detail by X-ray diffraction,X-ray photoelectron spectroscopy and X-ray absorption spectroscopy.The catalytic property was strongly influenced by the Fe substitution.The relation between catalytic performance and the degree of Fe substitution was examined with regard to the structure and surface characteristics of the mixed oxides.The Fe-containing catalysts exhibited higher activity attributable to the possible(Fe2+,Mo6+) and (Fe3+,Mo5+)valency pairs,and the highest activity was observed for Sr2Mg0.2Fe0.8MoO6-δ.The enhancement of the catalytic activity may be correlated with the Fe-relating surface lattice oxygen species and was discussed in view of the presence of oxygen vacancies. 相似文献