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Pd-dispersed CuS hetero-nanoplates for selective hydrogenation of phenylacetylene

Nano Research 2016年第4期9卷 1209-1219页

作者： Yu Wang Zheng Chen Rongan Shen Xing Cao Yueguang Chen Chen Chen Dingsheng Wang Qing Peng Yadong Li Department of Chemistry and Collaborative Innovation Center Nanomatefial Science and Engineering Tsinghua University Beijing 100084 China

We have exploited a new and distinctive combination method that ＂disperses＂ elemental Pd into CuS nanoplates. Pd was successfully dispersed by means of the concomitant transformation of CuS into an amorphous sulfide, which formed an intimate metal-sulfide contact via cation exchange and underwent a subsequent reduction. A series of such Pd-dispersed CuS hetero-nanoplates were synthesized with tailored proportions and compositions. By efficient utilization of noble metal atoms and stable anchored active sites, the optimal catalytic performance for the semihydrogenation of phenylacetylene, a probe reaction, was achieved with high selectivity, activity, and stability. We believe that the synthetic strategy described in our study is a feasible means of developing effective metal-sulfide catalysts for organic reactions.

关键词： palladium metal-sulfide hetero-nanoplates amorphous hydrogenation

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Photocatalytic hydrogenation of nitroarenes using Cu1.94S-Zn0.23Cd0.77S heteronanorods

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Nano Research 2018年第7期11卷 3730-3738页

作者： Zhanjun Yu Zheng Chen Yueguang Chen Qing Peng Rui Lin Yu Wang Rongan Shen Xing Cao Zhongbin Zhuang Yadong Li Department of Chemistry Tsinghua University Beijing 100084 China Faculty of Science Beijing University of Chemical Technology Beijing 100029 China Beijing Advanced Innovation Center for Soft Matter Science and Technology Beijing University of Chemical Technology Beijing 100029 China

Catalytic hydrogenation is an important process in the chemical industry. Traditional catalysts require the effective cleavage of hydrogen molecules on the metal-catalyst surface, which is difficult to achieve with non-noble metal catalysts. In this work, we report a new hydrogenation method based on water/ proton reduction, which is completely different from the catalytic cleavage of hydrogen molecules. Active hydrogen species and photo-generated electrons can be directly applied to the hydrogenation process with Cu1.94S-Zn0.23Cd0.775 semiconductor heterojunction nanorods. Nitrobenzene, with a variety of substituent groups, can be efficiently reduced to the corresponding aniline without the addition of hydrogen gas. This is a novel and direct pathway for hydrogenation using non-noble metal catalysts.

关键词： photocatalytic hydrogenation nitroarene selectivity heteronanorods

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Interface-induced formation of onion-like alloy nanocrystals by defects engineering

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Nano Research 2016年第2期9卷 584-592页

作者： Wei Jia Yuen Wu Yifeng Chen Dongsheng He Jinpeng Li Yu Wang Zhuo Wang Wei Zhu Chen Chen Qing Peng Dingsheng Wang Yadong Li Department of Chemistry and Collaborative Innovation Center for Nanomaterial Science and Engineering Tsinghua UniversityBeijing 100084 China Center of Advanced Nanocatalysis University of Science and Technology of China (CAN-USTC) Hefei 230026 China

The ability to controlled introduction of defects, particularly twin defects in Pt-based nanocrystals （NCs） provides a possibility to regulate the performance of Pt-based nanocatalyst. However, because of the high internal strain energy existed in twinned structures, the fabrication of defects in Pt-based NCs is sufficiently challenging. Here we demonstrate a ＂low-temperature interface-induced assembly＂ approach that provides precise control over Pt-Cu nanoparticles assembled at the hexadecylamine/water interface, yielding onion-like Pt-Cu NCs exposed a high density of twin defects. Moreover, a bending mechanism is proposed to elucidate the appearance of twin defects and lattice expanding （contraction） based on aberration corrected scanning transmission electron microscopy analysis. This work opens new routes to engineer defects in metal- based alloy NCs, enabling more opportunities in catalysis.

关键词： alloy nanocrystals assembly electroxidation twin defects interface

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Synthesis of palladium and palladium sulfide nanocrystals via thermolysis of a Pd–thiolate cluster

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Science China Materials 2015年第12期58卷 936-943页

作者：冯泉辰王威扬张永臻王定胜彭卿李金鹏陈晨李亚栋 Department of Chemistry and Collaborative Innovation Center for Nanomaterial Science and Engineering Tsinghua University

A novel one-pot approach to synthesize the tiara-like Pd(II) thiolate complex compound, [Pd(SCH_3)_2]_6, was developed. In this strategy, dimethyl sulfoxide(DMSO) was used as a thiolate source instead of methyl mercaptan(CH_3SH). DMSO was first decomposed into CH_3SH and formaldehyde(HCHO); then, the in situ as-formed CH_3SH molecules reacted with palladium acetate, and formed [Pd(SCH_3)_2]_6. By tuning the reaction condition, the morphology of the [Pd(SCH_3)_2]_6 assemblies can change from microprism to nanosphere. The characterization of the pyrolysis product demonstrated that these two kinds of [Pd(SCH_3)_2]_6 assemblies with different shapes could further decompose into palladium or palladium sulfides through different pyrolysis conditions.

关键词： Pd 团簇 SCH 二甲基亚砜甲硫醇硫氢甲烷金属钯

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