TRANSACTIONS OF TIANJIN UNIVERSITY
·
2019
·Vol. 25
·期 6
·595-602
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IF 0
Wang Nan,Ma Qingqing,Yuan Enxian,Wang Li
SBA-15 silica was synthesized by adding normal paraffin and alkyl benzene as swelling agents and using a low-temperature gelation procedure. Pd was then impregnated on SBA-15, yielding a catalyst. Characterizations of the catalyst by X-ray diffraction, N 2 adsorption/desorption, scanning electron microscopy, transmission electron micrographs, X-ray photoelectron spectroscopy, in situ FTIR, and a hydrogenation test of 2-ethyl-anthraquinone reveal that the addition of C 6 ‒C 9 normal paraffin and 1,3,5-triisopropylbenzene could enlarge the pore diameter without a significant loss of ordered structure. Moreover, the length of SBA-15 pore channels decreased significantly. However, the sizes of Pd particles increase as the pore diameter is enlarged. The largest pore size (13.6 nm) and short length of pore channels (ca. 0.35 μm) are achieved by adding n-hexane. As a result, this catalyst exhibits the highest hydrogenation activity with an approximately 100% improvement, compared with a conventionally synthesized catalyst in the absence of a swelling agent.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Xiao-Chen Ma,Chun Pu,Yue-Xing Zhang,Gang-Gang Chang,Ge Tian,Si-Ming Wu,Jia-Wen Liu,Zhi-Yi Hu,Li-Ying Wang,Yi-Xia Yin,Christoph Janiak,Xiao-Yu Yang
Efficient regeneration of Pd catalysts is a challenge and has a very high technological importance. Herein, we report confined Pd clusters with the ultrafine size (1.2 nm) and ultralow loading amount (0.14 wt%) in a metal–organic framework (MOF), which could potentially allow for the successive realization of the cascade-type catalytic reaction from starting reagents to final desired products, and thus to avoid the excessive processes, save energy and reduce waste. Experiments and theoretical computations have been conducted to study the strong host–guest interaction between the Pd clusters and the MOF support, leading to the high catalytic activity and dynamic of the Pd clusters. A unique dynamic structure from active disordered arrangement to deactive crystalline arrangement and then back to the active disordered arrangement (>99% of activity after regeneration by simple H 2 reduction). The MOF-confined Pd shows excellent catalytic activity (>99% activity), selectivity (around 100%) and stability (>99% activity after recycling) under mild reaction conditions (atmospheric temperature and pressure).
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JOURNAL OF NANOBIOTECHNOLOGY
·
2021
·Vol. 19
·期 1
·1-14
·
IF 10.435
Guo Xiaoyang,Liu Jia,Jiang Lingdong,Gong Wanjun,Wu Huixia,He Qianjun
Background Photothermal therapy (PTT) frequently cause thermal resistance in tumor cells by inducing the heat shock response, limiting its therapeutic effect. Hydrogen sulfide (H2S) with appropriate concentration can reverse the Warburg effect in cancer cells. The combination of PTT with H2S gas therapy is expected to achieve synergistic tumor treatment.Methods Here, sulourea (Su) is developed as a thermosensitive/hydrolysable H2S donor to be loaded into Pd nanocubes through in-depth coordination for construction of the Pd-Su nanomedicine for the first time to achieve photo-controlled H2S release, realizing the effective combination of photothermal therapy and H2S gas therapy.Results The Pd-Su nanomedicine shows a high Su loading capacity (85 mg g−1), a high near-infrared (NIR) photothermal conversion efficiency (69.4%), and NIR-controlled H2S release by the photothermal-triggered hydrolysis of Su. The combination of photothermal heating and H2S produces a strong synergetic effect by H2S-induced inhibition of heat shock response, thereby effectively inhibiting tumor growth. Moreover, high intratumoral accumulation of the Pd-Su nanomedicine after intravenous injection also enables photothermal/photoacoustic dual-mode imaging-guided tumor treatment.Conclusion sThe proposed NIR-responsive heat/H2S release strategy provides a new approach for effective cancer therapy.Graphic abstract
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JOURNAL OF MATERIALS SCIENCE
·
2019
·Vol. 55
·期 4
·1525-1535
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IF 3.442
Zhang Jian,Jiang Yuting,Zhang Jiaxin,Zhang Lanhe,Wang Bing,Li Zheng,Liu Congze,Wang Haonan
2,4-Dichlorophenol (2,4-DCP) is a kind of toxic organic compound listed as a priority pollutant by the environmental protection agency, which will endanger the environment and human health. The accumulation of 2,4-DCP in the environment has become a serious problem today since 2,4-DCP is difficult to be degraded by traditional methods. In this study, a novel palladium/graphene oxide/indium tin oxide (Pd/GO/ITO) composite electrode was prepared by constant current electrodeposition method. And the surface morphology, crystal structure and surface element valence state of the electrode were observed and analyzed by SEM, XRD and XPS, respectively. Finally, by studying the influence of different conditions on the performance of the electrodes, the electrochemical degradation efficiency of the new electrodes on 2,4-DCP was investigated. It was found that the degradation of the Pd/GO/ITO electrodes on 2,4-DCP followed a quasi-first-order reaction under different conditions.
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Particuology
·
2019
·
IF 2.616
Jian Zhang,Liang Wang,Fang Chen,Feng-Shou Xiao
Product selectivity adjustment is a much-studied topic in mesoscience that is critical for industrial processes and strongly related to reaction intermediates formed by interactions between catalytic active sites and reactants. Herein, we report efficient adjustment of the product selectivity in the hydrogenation of substituted nitroarenes via rational reaction intermediates achieved using controllable Pd nanoparticles. Pd nanoparticles fixed within zeolite Beta crystals (Pd@Beta) afforded rational Pd–NO 2 interactions, in which the Pd nanoparticle-adsorbed substituted nitroarenes, such as nitrobenzaldehyde, were reasonably hydrogenated into the corresponding aminobenzaldehyde. However, for Pd nanoparticles supported on the external surfaces of zeolite beta crystals, various side products were obtained owing to the coexistence of Pd NO 2 and Pd C O interactions. When Pd nanoparticles were artificially controlled in various positions in a fixed-bed reactor, the product selectivity was significantly affected. These results demonstrate the importance of molecular adsorption and diffusion processes in adjusting product selectivity in catalytic reactions.
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Journal of the American Chemical Society
·
2019
·
IF 14.695
Yonggang Feng,Weiwei Xu,Bolong Huang,Qi Shao,Lai Xu,Shize Yang,Xiaoqing Huang
The pursuit of efficient hydrogenation nanocatalysts with a desirable selectivity toward intricate substrates is state-of-the-art research but remains a formidable challenge. Herein, we report a series of novel PdCdx nanocubes (NCs) for ultraselective hydrogenation reactions with flexible tuning features. Obtaining a desirable conversion level of the substrates (e.g., 4-nitrophenylacetylene (NPA), 4-nitrobenzaldehyde (NBAD), and 4-nitrostyrene (NS)) and competitive selectivity for all potential hydrogenation products have been achieved one by one under optimized hydrogenation conditions. The performance of these PdCdx NCs displays an evident dependence on both the composition and the use of Cd and a need for a distinct hydrogen source (H2 or HCOONH4). Additionally, for the selectivity of hydrogen to be suitably high, the morphology of the NCs has a very well-defined effect. Density functional theory calculations confirmed the variation of adsorption energy for the substrate and hydrogenation products by carefully controlled introduction of Cd, leading to a desirable level of selectivity for all potential hydrogenation products. The PdCdx NCs also exhibit excellent reusability with negligible activity/selectivity decay and structural/composition changes after consecutive reactions. The present study provides an advanced strategy for the rational design of superior hydrogenation nanocatalysts to achieve a practical application for desirable and selective hydrogenation reaction efficiency.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Yunlong Guo,Yijing Gao,Xiang Li,Guilin Zhuang,Kuncan Wang,Yi Zheng,Daohua Sun,Jiale Huang,Qingbiao Li
Pd nanoparticles (NPs)-based catalysts were synthesized, characterized and used to catalyze the oxidation of volatile organic compound (VOC) pollutants. A biogenic method was employed to synthesize Pd NPs with tunable sizes by using Cacumen platycladi (CP) leaf extract as a reducing agent. The Pd NPs were then anchored over a support which was made from KIT-6-templated three-dimensionally ordered mesoporous (3DOM) CeO 2 (i.e., kit-CeO 2 ) to form xPd/kit-CeO 2 catalysts with various Pd loadings (x denotes Pd loading, wt%). The physicochemical properties such as morphology, structure and elemental distribution of the xPd/kit-CeO 2 catalysts and the support were comprehensively characterized. The BET surface areas of the support and catalysts varied in the range of 105–109 m 2 /g. In the benzene oxidation catalyzed by 0.5Pd/kit-CeO 2 , the temperature required for 90% benzene conversion was significantly reduced to 187 °C, compared with the published results. Furthermore, the 0.5Pd/kit-CeO 2 showed stable catalytic activity after being used for 150 h in on-stream reaction. Besides, density functional theory calculation indicated that the synergetic effects of Pd NPs and the kit-CeO 2 support would facilitate the activation of benzene adsorbed on Pd NPs prior to oxidation. The catalytic performance of 0.5Pd/kit-CeO 2 correlated well with the features of CP leaf extract, high Pd 0 concentration, abundant oxygen adspecies, low temperature reducibility, and strong interactions between Pd NPs and kit-CeO 2 support. The biogenic method is better than the chemical method to synthesize Pd NPs with higher catalytic activity while the kit-CeO 2 is better than the commercial CeO 2 and KIT-6-templated transition metal oxides (e.g., Fe 2 O 3 and Co 3 O 4 ) as a supporting material.
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Journal of the Taiwan Institute of Chemical Engineers
·
2018
·
IF 3.849
Fengxia Wang,Xiaobo Niu,Wei Wang,Wangli Jing,Yulong Huang,Ji Zhang
A green innovation strategy is performed to synthesize palladium nanoparticles (Pd NPs) using Cynomorium songaricum polysaccharide (CSP). The structure and properties of the as-prepared Pd NPs are characterized by a set of techniques, including transmission election microscopy, X-ray photoelectron spectroscopy, powder X-ray diffraction and cyclic voltammetry. The results show that Pd NPs are well dispersed with a mean size of 4.2 nm. As-obtained Pd–CSP/C electrode exhibits good stability and anti-interference ability for glucose detection in electrochemical studies. It can completely cover the normal blood glucose concentration with high sensitivities of 17.7 µA mM −1 cm −2 , and excellent stability during long-term electrochemical detection. Compared with the commercial glucometer, the relative deviation of the measured samples was equal to 5.0%. Significantly, this study offers an environmental friendly polysaccharide way for fabricating nanomaterials, which would develop more nanomaterials for various application fields in future.
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APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING
·
2015
·Vol. 119
·期 2
·603-608
·
IF 1.704
Zhang Yulong,Xu Zhizhen,Sun Huanghui,Qiu Qiaoli,Zhang Lingfan,Xia Wei,Zhang Wenqing
In this study, we have constructed nano-sized hollow carbon spheres with large cavities and thin shells under hydrothermal conditions using ricinoleic acid as the soft template and 2,4-dihydroxybenzoic acid and hexamethylenetetramine as the sphere precursors. After being filled with Fe particles and loaded with Pd particles, the spheres became magnetic, allowing easy separation from the liquid phase by a magnet, and showed excellent catalytic performance in decomposing formic acid. The hollow carbon spheres and the magnetic catalysts were characterized by TEM, FE-SEM, XPS, and FTIR.
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CHEMOSPHERE
·
2015
·
IF 3.34
Ya-Li Chen,Lu Xiong,Xiang-Ning Song,Wei-Kang Wang,Yu-Xi Huang,Han-Qing Yu
Electrocatalytic hydrodehalogenation is a cost-effective approach to degrade halogenated organic pollutants in groundwater, and Pd-based catalysts have been found to be an efficient cathode material for this purpose. In this work, a novel Cu@Pd bimetallic catalyst loaded on Ti plate was prepared via combined electrodeposition and galvanic replacement for electrocatalytic hydrodehalogenation of atrazine, a typical halogenated pollutant. The obtained bimetallic catalyst with uniformly dispersed Pd nanoparticles possessed a large electrochemically active surface area of 572 cm 2 . The Cu@Pd/Ti cathode exhibited a higher electrocatalytic efficiency towards atrazine reduction than the individual Pd/Ti or Cu/Ti cathodes, and achieved up to 91.5% within 120 min under a current density of 1 mA cm −2 . Such an electrocatalytic reduction followed pseudo-first-order kinetics with a rate constant of 0.0214 min −1 . Atrazine was selectively transformed to dechlorinated atrazine, and its degradation pathway was identified. Current density was found to have a critical influence on the atrazine reduction due to the competitive hydrogen evolution reaction at a higher current density. The fabricated bimetallic catalyst also exhibited a good stability. This work provides an efficient and stable electrocatalyst for chlorinated contaminate removal and groundwater remediation.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2016
·
IF 3.014
Xiaomeng Li,Ming Wen,Dandan Wu,Qingsheng Wu,Jiaqi Li
For the exploration of catalysts with excellent performance in alkaline fuel cells, high-performance two-dimensional (2D) Pd-on-NiCu nanosheets were synthesized through the kinetics controlling synthesis of NiCu nanosheets followed by Pd nanoparticles (NPs) embedding treatment at room temperature. In which case, well-dispersed Pd NPs with the average diameter of ∼4 nm are embedded on NiCu nanosheets (BET surface area of 180.7 m 2 g −1 ). Pd-on-NiCu nanosheets exert remarkable high performance in electrocatalytic activity, methanol-tolerance and stability, the electrocatalytic mass activity of Pd-on-NiCu nanosheets is 1827 mAmg −1 , which is over 6-fold higher than that of commercial Pd/C (289 mAmg −1 ), and the current density of the electrocatalyst decreases after 300 cycles of only 6%. Therefore, Pd-on-NiCu nanosheets can be considered as one of the most promising candidates for fuel cells applications.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2016
·
IF 3.205
Qizhi Dong,Meiling Huang,Cancheng Guo,Gang Yu,Mimi Wu
There is significant interest in developing new catalyst supports such as metal carbides to overcome the electrochemical corrosion problem of traditional high surface area carbon. A key challenge is the dispersion and stability of the catalysts on the non-carbon based materials. This paper reports a new approach to functionalize titanium carbide by poly (diallyldimethylammonium chloride) (PDDA), investigated as a new catalyst support for Pd catalyzed electrochemical reaction . Thermal gravimetric analysis confirmed the successful noncovalent functionalization of TiC by PDDA. Pd nanoparticles are deposited in situ on the PDDA-wrapped TiC surface through electrostatic interactions mechanism. According to transmission electron microscopy (TEM) observations, Pd nanoparticles with a mean size of ∼2.9 nm are homogeneously deposited on TiC(P). Among all the samples tested, the Pd/TiC(P) catalysts exhibit the highest resistance to CO poisoning, catalytic activity and stability towards formic acid electrooxidation . This performance was attributed to a strong Pd↔TiC interaction and the formation of oxygenated species on the TiC.
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