RSC Advances
·
2014
·Vol. 4
·期 58
·30914-30922
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IF 3.708
Mingxi Chen,Zhe Zhang,Lingzhi Li,Yu Liu,Wei Wang,Jianping Gao
Ultrafine Ag–Pd bimetallic nanoparticles homogeneously distributed on reduced graphene oxide (rGO) were prepared by redox reactions between Pd2+, Ag+ and GO. This method is simple, and the use of rGO as a support facilitated the separation and reuse of the Ag–Pd@rGO catalyst. The Ag–Pd@rGO bimetallic nanoparticles were characterized by ultraviolet-visible spectroscopy, Raman spectroscopy, thermogravimetric analysis, X-ray diffraction analysis, and X-ray photoelectron spectroscopy. The microstructure of the Ag–Pd@rGO was investigated with scanning electron microscopy and transmission electron microscopy. The Ag–Pd@rGO catalyst exhibited high catalytic activities in the Suzuki-Miyaura carbon coupling reaction and the Sonogashira carbon coupling (SCC) reaction. These reactions used mild, efficient, ligand-free and heterogeneous conditions. Interestingly, the presence or absence of oxygen in the SCC catalytic system resulted in two different products, in which oxygen can be used as “switch” to control different products.
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ChemSusChem
·
2015
·Vol. 8
·期 10
·1761-1767
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IF 7.657
Yi Shao,Qineng Xia,Xiaohui Liu,Guanzhong Lu,Yanqin Wang
Graphical Mild mannered: Under mild conditions (170 °C, 2.5 MPa), Pd/10 %Nb 2 O 5 /SiO 2 is effective for the hydrodeoxygenation reactions of 4-(2-furyl)-3-buten-2-one (the aldol adduct of furfural with acetone), palmitic acid, tristearin, and diphenyl ether (model compounds of vegetable oils, microalgae oils, and lignin) and gives high yields (>94 %) of alkanes with little C C bond cleavage. A simple Pd-loaded Nb 2 O 5 /SiO 2 catalyst was prepared for the hydrodeoxygenation of biomass-related compounds to alkanes under mild conditions. Niobium oxide dispersed in silica (Nb 2 O 5 /SiO 2 ) as the support was prepared by the sol–gel method and characterized by various techniques, including N 2 adsorption, XRD, NH 3 temperature-programmed desorption (TPD), TEM, and energy-dispersive X-ray spectroscopy (EDAX) atomic mapping. The characterization results showed that the niobium oxide species were amorphous and well dispersed in silica. Compared to commercial Nb 2 O 5 , Nb 2 O 5 /SiO 2 has significantly more active niobium oxide species exposed on the surface. Under mild conditions (170 °C, 2.5 MPa), Pd/10 %Nb 2 O 5 /SiO 2 was effective for the hydrodeoxygenation reactions of 4-(2-furyl)-3-buten-2-one (aldol adduct of furfural with acetone), palmitic acid, tristearin, and diphenyl ether (model compounds of microalgae oils, vegetable oils, and lignin), which gave high yields (>94 %) of alkanes with little C C bond cleavage. More importantly, owing to the significant promotion effect of NbO x species on C O bond cleavage and the mild reaction conditions, the C C cleavage was considerably restrained, and the catalyst showed an excellent activity and stability for the hydrodeoxygenation of palmitic acid with almost no decrease in hexadecane yield (94–95 %) in a 150 h time-on-stream test.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2015
·
IF 3.313
Hansheng Wan,Qizhi Dong,Guiming Zhu,Gang Yu,Tianwu Yin,Meiling Huang
In this work, anatase-TiO 2 is investigated as a catalyst support in Pd/TiO 2 –C composite to improve the electrocatalytic properties of Pd for formic acid oxidation reaction (FAOR). Pd/TiO 2 has been synthesized by an impregnation-reduction method and then mixed with Vulcan XC-72R carbon black to obtain Pd/TiO 2 –C composite. Transmission electron microscopy (TEM) images show Pd nanoparticles (ca.3.5 nm in average diameter) in the Pd/TiO 2 –C (1:1) composite catalyst were dispersed on the surface of TiO 2 with a narrow particle size distribution . Electrochemical tests demonstrate Pd/TiO 2 –C (1:1) composite has significantly increased catalytic activity and stability compared with Pd/C for FAOR. The proposed reasons for these observations are the excellent acid corrosion and oxidation resistance of TiO 2 and the synergistic effect of Pd and TiO 2 nanoparticles . The effect of mass ratios of TiO 2 to C on the catalytic performance is also discussed. The best catalytic activity and stability for FAOR is found when the mass ratio of TiO 2 to C is 1:1. It can be interpreted as the synergistic effects and conductivity reach balance at this point.
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ACS Applied Materials & Interfaces
·
2015
·
IF 6.723
Tao Yang,Guojian Cao,Qingli Huang,Yanxia Ma,Sheng Wan,Hong Zhao,Na Li,Xia Sun,Fujun Yin
Exploring superior catalysts with high catalytic activity and durability is of significant for the development of an electrochemical device involving the oxygen reduction reaction. This work describes the synthesis of Pt-on-Pd bimetallic heterogeneous nanostructures, and their high electrocatalytic activity toward the oxygen reduction reaction (ORR). Pt nanoclusters with a size of 1–2 nm were generated on Pd nanorods (NRs) through a modified Cu underpotential deposition (UPD) process free of potential control and a subsequent surface-limited redox reaction. The Pt nanocluster decorated Pd nanostructure with a ultralow Pt content of 1.5 wt % exhibited a mass activity of 105.3 mA mg–1 (Pt–Pd) toward ORR, comparable to that of the commercial Pt/C catalyst but 4 times higher than that of carbon supported Pd NRs. More importantly, the carbon supported Pt-on-Pd catalyst displays relatively small losses of 16% in electrochemical surface area (ECSA) and 32% in mass activity after 10 000 potential sweeps, in contrast to respective losses of 46 and 64% for the commercial Pt/C catalyst counterpart. The results demonstrated that Pt decoration might be an efficient way to improve the electrocatalytic activity of Pd and in turn allow Pd to be a promising substitution for commercial Pt catalyst.
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RSC Advances
·
2015
·Vol. 5
·期 124
·102811-102817
·
IF 3.84
Fengwei Zhang,Shuai Chen,Huan Li,Xian-Ming Zhang,Hengquan Yang
A multi-component mesoporous core–shell structured nanocatalyst was prepared via encapsulation of a hydrophobic mesoporous carbon with amino-functionalized mesoporous silica, followed by coordination of palladium precursors and then reduction with a NaBH4 reagent. The resulting Pd/MCN@MS-NH2 catalyst could be well-dispersed in an aqueous medium owing to the inherent hydrophilic properties of the mesoporous silica shell. The experimental results indicated that the Pd/MCN@MS-NH2 catalyst had high catalytic activity and selectivity for the hydrogenation of phenol to cyclohexanone under 1 atm of H2 at 80 °C for 3 h in pure water (conversion > 99% and selectivity 99%). Furthermore, the catalyst can be easily recovered and reused six times without significant loss of catalytic activity.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Jinglei Cui,Yujun Cui,Jingjing Tan,Huirong Zhang,Mengyuan Gu,Long Huang
Volatile organic compounds (VOCs) are one of the main pollutants produced in industrial processes. Catalytic oxidation is an effective method to eliminate VOCs, and the key lies in designing efficient metal catalyst. In this work, Pd-Pt/SiO 2 bimetallic catalysts were designed and prepared by the immobilization method, and their performances for toluene oxidation were evaluated. The addition of Pt into the catalyst elevated markedly the reduction of Pd active sites, leading to abundant electron-deficient Pd 0 and electron-rich Pt 0 in the Pd 2 Pt 1 catalyst, which were confirmed by TEM, CO pulse adsorption and in-situ XPS. As revealed by O 2 -TPD and toluene-TPD characterization, the cooperative effect of electron-deficient Pd 0 and electron-rich Pt 0 in Pd 2 Pt 1 catalyst facilitated the activation of O 2 and toluene, thus enhanced greatly its activity. A conversion of 90% (T 90 ) for toluene was achieved over Pd 2 Pt 1 catalyst at 165 ℃, and the apparent activation energy ( E a ) over Pd 2 Pt 1 catalyst was lower than that over other Pd-Pt bimetallic and monometallic Pd or Pt catalysts. Additionally, the reaction mechanism was studied by In - situ DRIFTS, the results showed that the toluene oxidation passed successively benzyl alcohol, benzaldehyde, benzoic acid and maleic anhydride , then maleic anhydride was further oxidized to CO 2 and water.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhefei Zhao,Xuyao Yao,Ruopeng Yu,Xingyu Luo,Minhao Chen,Xiangxiang Zhang,Yinghua Xu,Youqun Chu,Xinbiao Mao,Huajun Zheng
Electrocatalytic hydrodechlorination (EHDC) stands out as an economical and prospective technology for eliminating chlorinated organic pollutants. Single-atom catalyst engineering and metal-support interaction (MSI) offer the promising strategies for developing electrocatalysts with high atom utilization and reactivity. Herein, atomically dispersed palladium (Pd) anchored on the iron (Fe)-introduced nickel phosphide (NiFeP) support is reported. The prepared NiFeP-Pd electrode exhibits outstanding electrocatalytic activity in 4-CP removal efficiency (98.8 %) with an ultra-low dosage of Pd (0.0497 mg cm −2 ) and the highest reported MA value (446.01 min −1 g −1 ), surpassing Ni 2 P-Pd by 6.34 times. Experimental results combined with theoretical calculations suggest that the superior performance of NiFeP-Pd stems from the modulated support by Fe introduction, which not only enhances the generation of adsorbed atomic hydrogen species (H*), but also reduces the energy barrier of C-H formation on Pd sites by regulating the MSI. In addition, single-Pd-atom construction on NiFeP with good conductivity and large specific surface area makes the contributions as well.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Ruiting Li,Tengyang Gao,Yao Wang,Yan Chen,Wen Luo,Yang Wu,Yu Xie,Yong Wang,Yifan Zhang
The application of metal catalysis has gained prominence as a study area in recent years. In this work, we use adsorptive reduction and calcination to create Au–Pd alloy catalysts on COCN-2 with varying metal loadings. The plasma resonance effect of the alloys increases the photoresponse of the catalysts, and the engineering of nitrogen defects strengthens the strong bonds between Au–Pd alloy particles and carbon nitride graphite, optimizing the electronic structure, encouraging electron-directed migration, and increasing the efficiency of the reduction reaction. As a result, the efficiency of hydrogen generation by the Au–Pd 0.6 /COCN-2 catalyst is 5.089 mmol g −1 h −1 , which is 2367 times higher than that of the g-C 3 N 4 catalyst. Our findings highlight the crucial part that flaws play in strengthening the strong bonds that exist between the metal and the support, which enhances photocatalytic hydrogen generation. This work offers insightful information about creating effective photocatalysts.
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ChemistrySelect
·
2024
·Vol. 9
·期 41
·e202402898
·
IF 1.9
Yuxian Wang,Pengfei Bai,Xian Sheng,Molan Qing,Yuanyang Yi,Zhidong Zhang,Ling Jiang,Liying Zhu
Graphical This study reports an environmentally friendly approach for the extracellular synthesis of Pd−Ag bimetallic nanoparticles (Pd−Ag BNPs) with small size by reduction of Pd and Ag ions using cell-free supernatant of Deinococcus wulumuqiensis . The application of as-prepared bionanocatalyst in catalytic degradation of pollutant dyes demonstrates that Pd−Ag BNPs have excellent degradation ability of 4-nitrophenol and Rhodamine. Catalytic reduction of organic pollutants using metal nanoparticles (MNPs) as nanocatalyst is a promising approach. The widespread application of MNPs have led to an increase demand for their production. The green biosynthesis of MNPs using microbes is becoming increasingly important as they are benign and environmentally friendly. In this work, Deinococcus wulumuqiensis ( D. wulumuqiensis ) with high resistance to stresses was applied for the green preparation of different MNPs, including palladium nanoparticles (Pd NPs), silver nanoparticles (Ag NPs), and Pd−Ag bimetallic nanoparticles (Pd−Ag BNPs). The resultant MNPs exhibited a face-centered cubic structure, with average size of 6.70 (Pd NPs), 6.24 (Ag NPs), and 6.13 nm (Pd−Ag BNPs), respectively. FT-IR spectra indicated that the proteins and polysaccharides expressed by D. wulumuqiensis could potentially contributed to the formation of MNPs. The application of as-prepared biocatalyst in catalytic degradation of pollutant dyes demonstrated that Pd−Ag BNPs had greater degradation ability of 4-nitrophenol (95.1 %) and Rhodamine B (85.1 %) than monometallic nanoparticles. The pseudo-first-order kinetics results further indicated the superior catalytic ability of Pd−Ag BNPs, with rate constant of 0.450±0.009 (4-nitrophenol) and 1.54×10 −2 min −1 (Rhodamine B), respectively. Thus, the present study confirms that D. wulumuqiensis represents a promising candidate for the biosynthesis of Pd-based nanoparticles with small size, which exhibited potential applications as bionanocatalyst in the degradation of water pollutants.
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INORGANIC CHEMISTRY COMMUNICATIONS
·
2024
·
IF 4.4
Peng Song,Shutong Hou,Bo Gong,Jingjing Zhao,Mingcong Zhu,Hui Liu,Hui Zhao,Tao Wu,Xixi Zhu,Qingyun Liu
Tetracycline (TC) is extensively employed as a broad-spectrum antibacterial agent, and its byproducts have been identified in a variety of water bodies, posing a significant risk to both aquatic ecosystems and human health. Among the prevalent techniques for treating water contaminants, photodegradation stands out. In this research, we synthesized a novel nanocomposite material, embedding bimetallic nanoparticles onto halloysite nanotubes (HNT) (Pd@Ni/N-HNT), aimed at photocatalytically degrading TC. The Pd@Ni/N-HNT demonstrated the capability to enhance the TC degradation efficiency to 100 % under visible light for a duration of 120 min, effectively doubling the performance of pure H 2 O 2 degradation. The influence of pH levels in aquatic environments on the TC degradation efficiency was explored. Through electron spin resonance (EPR) studies and free radical scavenging tests, it was verified that •O 2 − and h + are pivotal in the degradation process. Furthermore, Pd@Ni/N-HNT showcased effective degradation capabilities in both tap and river water, achieving degradation rates exceeding 70 % in 120 min and 95 % in 180 min, respectively. This investigation not only sheds light on the potential of utilizing Pd@Ni/N-HNT as a potent catalyst for the photocatalytic degradation of TC but also offers a comprehensive framework for the future development of nanomaterials aimed at the environmental remediation of organic pollutants. The findings herein provide a pivotal reference and guide for advancing the application of nanotechnology in the purification of water, thereby contributing to the safeguarding of aquatic ecosystems and public health.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Qian Guo,Ziyun Su,Dong Xiang,Beirong Yu,Di Wang,Youjun Fan,Fuqin Zheng,Wei Chen
As model catalysts, it is necessary to study the relationship between the structure and properties of ultra-small metal nanoclusters (MNCs) and to reduce their steric hindrance as much as possible, e.g. preparing ultrasmall MNCs protected by ultra-short ligands. However, it is challenging to attain various MNCs with the same cores but different surface stabilizing ligands. Additionally, shortening the chains of protecting ligands will lead to larger MNC cores. Here, four different Pd NCs (Pd 6 (SC 4 H 9 ) 12 , Pd 6 (SC 8 H 17 ) 12 , Pd 6 (SC 6 ( C 2 )H 17 ) 12 and Pd 6 (SC 6 H 13 ) 12 ) were successfully synthesized by a slow synthesis process. All these clusters consist of six Pd atoms and are stabilized by 12 thiols with different chain lengths and steric hindrance. The catalytic properties of the as-prepared Pd 6 NCs were evaluated using the catalytic reduction of p-nitroaniline to p-phenylenediamine as a model reaction. The outcomes indicated that shortening the chain length of the protecting thiols could enhance the catalytic activity of the Pd 6 NCs. Notably, stable and active ultra-small Pd 6 clusters stabilized by ultra-short ligands (HSC 4 H 9 ) were successfully synthesized. Although the performance of Pd 6 (SC 4 H 9 ) 12 clusters protected by the ultra-short thiols is lower than that of commercial palladium on carbon (Pd/C), they display higher stability. Interestingly, the activity of Pd 6 NCs protected by ethyl-branched alkane thiols is also better than that of Pd 6 NCs protected by the alkane thiol ligands with the same chain length or the same number of carbon numbers. This work provides clear evidence that the catalytic activity of atomically precise MNCs can be controlled by regulating the surface stabilizing ligands.
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INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Changjin Xu,Yinglei Liu,Huiqing Guo,Chun Du,Gaowu Qin,Song Li
The ability to finely tune the nuclearity of active metal sites is critical for designing highly selective catalysts, especially for hydrogenation processes. In this work, we developed a novel PdCu catalyst with an ordered body-centered cubic (BCC) structure, enabling precise control over Pd nuclearity to optimize selectivity. Using a facile polyol synthesis method, we modulated the Pd coordination environment, reducing the Pd–Pd coordination number from 3 (disordered face-centered cubic, FCC) to 0 (ordered BCC), thereby achieving full isolation of Pd by the surrounding Cu atoms. This structural transformation enhances hydrogen spillover and weakens ethylene adsorption, resulting in superior activity for the selective hydrogenation of acetylene to ethylene. The ordered PdCu supported on Al2O3 (o-PdCu/Al2O3) achieved a 99% acetylene conversion with an 84.5% ethylene selectivity at near-room temperature. This work highlights the importance of controlling atomic-scale nuclearity in metal catalysts and provides a promising strategy for improving the catalytic efficiency and selectivity in industrially significant processes.
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