ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Chunshan Lu,Qianwen Zhu,Xuejie Zhang,Haoke Ji,Yebin Zhou,Hao Wang,Qiangqiang Liu,Juanjuan Nie,Wenfeng Han,Xiaonian Li
Achieving high selectivity is one of the major challenges for the noble metal catalysts. A strategy of decoration of Pd nanoparticles by N–S doped carbon quantum dots (N,S-CQDs) to regulate selectivity is proposed. Through adjusting the loading amounts of N,S-CQDs, high selectivity toward catalytic hydrogenation reactions can be obtained. N,S-CQDs facilely adhere to the Pd nanoparticle via surface reactions among C–S/C–N species of N,S-CQDs and C–O species of the carbon support under the catalysis of Pd particles. N loss was detected due to the transformation of some C–N species into nitrogen-containing soluble substances or gas. However, S-containing species, specially −SO2/SO3 species, are turned into C–S–C (thiophene-S), leading to a strong coordination between Pd and S. As a result, a N,S-CQDs-Pd interface is fabricated, in which electrons transfer from Pd to S species and the interface of Pd–S plays a major role in hydrogen spillover and generation of dissociated hydrogen with negative charge. Consequently, Pd@N,S-CQDs suppress the hydrodehalogenation and exhibit superior conversion and selectivity (both 100%) for the selective hydrogenation of various halonitrobenzenes. N,S-CQDs as a nonmetallic promoter of metal catalysts provides a promising strategy for the improvement of selectivity.
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ChemCatChem
·
2019
·Vol. 11
·期 9
·2362-2369
·
IF 4.495
Xue Zhao,Yunfan Fu,Chen Yao,Shuran Xu,Yu Shen,Qiong Ding,Wenjing Liu,Haibo Zhang,Xiaohai Zhou
Graphical A closo case : In situ preparation of ultrafine Pd and Pt nanoparticles on dodecahydro-closo-dodecaborate organic polymers for high efficiency catalytic hydrolytic dehydrogenation of ammonia borane. Using in situ reduction strategy by combining organic frameworks and ultrafine Pd and Pt nanoparticles (Pd−NPs and Pt−NPs) to synthesize composites with tunable morphology and high dispersion has attracted extensive attentions in fabrication of composite nanomaterials. Herein, on the new kind of substrate, BOPs@Pd and BOPs@Pt nano materials have been successfully fabricated via in situ reduction of Na 2 PdCl 4 and H 2 PtCl 6 triggered by reducibility of organic boron polymers (BOPs). The final products are obtained by loading Pd−NPs and Pt−NPs with ultra-small size and high dispersion without any tedious chemical modification or additional additives. These materials show high catalytic activity and recyclability in the hydrolysis dehydrogenation of ammonia borane (AB).
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Polymers
·
2018
·Vol. 10
·期 4
·437
·
IF 2.935
Bing Zhang,Shixing Wang,Likang Fu,Libo Zhang
A new adsorbent was prepared via modified poly(glycidyl methacrylate) with 8-aminoquinoline (AQ-PGMA) for the recovery of Pd(II) from solution. The practical application values of AQ-PGMA, including efficiency, selectivity and reusability for the recovery of Pd(II), are proved by the various experiment parameters. The parameters include HCl concentration, adsorption time, initial Pd(II) concentration, coexisting ions and reused cycles. The prepared AQ-PGMA showed a high adsorbing capacity for Pd(II) (up to 267.90 mg/g) when the concentration of HCl is higher than 0.4 mol/L. The analysis of the adsorption process indicated that the adsorption kinetics followed a pseudo-second-order kinetic model and the adsorption isotherms obeyed the Hill model. The Hill model showed that one adsorption site on the AQ-PGMA could combine 1.45 Pd(II). In addition, the obtained adsorbent demonstrated good regenerative ability and satisfying selectivity for the recovery of Pd(II). The adsorption mechanism was dominated by the chelation and ion exchange reactions between amines/hydroxyl groups and Pd(II). The experiments confirmed that AQ-PGMA was efficient for recovery of Pd(II) from highly acidic aqueous solutions.Keywords:adsorption;palladium;efficiency;selectivity;reusability
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高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2018
·Vol. 53
·期 19
·13912-13923
·
IF 2.993
Li Xin,Pu Zhilong,Zhou Hao,Zhang Wenchi,Niu Xiangheng,He Yanfang,Xu Xuechao,Qiu Fengxian,Pan Jianming,Ni Liang
In this work, we proposed a new hybrid of Pd nanoparticles dispersed on CeO 2 nanotubes (Pd NPs/CeO 2 NTs) with synergistically enhanced peroxidase-like activity for the visual detection of sulfhydryl compounds. In comparison with individual Pd NPs and CeO 2 NTs, the Pd NPs/CeO 2 NTs hybrid exhibited a synergy effect to trigger the oxidation of colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to its blue product TMBox mediated by H 2 O 2 . It was further demonstrated that the improved activity observed in Pd NPs/CeO 2 NTs originated from the strong interplays between Pd NPs and CeO 2 NTs, which could significantly increase the Ce 3+ /Ce 4+ ratio. Besides, sulfhydryl compounds were found to have the capacity to suppress the color reaction of TMB + H 2 O 2 catalyzed by the Pd NPs/CeO 2 NTs nanozyme at a low level. Based on this principle, mercaptoacetic acid in the concentration range of 66–400 nM could be linearly determined. Similarly, sulfhydryl-containing amino acid (cysteine) and its derivative (glutathione) in the linear scope of 6–40 nM were also detected, providing a detection limit down to 2.9 and 11.3 nM, respectively.
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NEW JOURNAL OF CHEMISTRY
·
2017
·Vol. 42
·期 3
·1771-1778
·
IF 3.269
Saisai Cheng,Xufeng Meng,Ningzhao Shang,Shutao Gao,Cheng Feng,Chun Wang,Zhi Wang
Well-dispersed Pd nanoparticles were anchored on g-C3N4 nanosheets, which were prepared by a liquid-phase exfoliation method. The hybrid material displayed excellent catalytic activity for the transfer hydrogenation of nitroarenes. The reactions can be conducted smoothly in water at room temperature with formic acid as hydrogen source. Aniline was produced in excellent yield (>99%; turnover frequency: 853), surpassing the majority of reported heterogeneous catalysts using formic acid or formates as hydrogen source. The increased activity of such a hybrid catalyst can be ascribed to the nitrogen-rich and amphipathic property of the carbon nitride support, the stable and uniform dispersed Pd nanoparticles and the Mott–Schottky effect between the g-C3N4 nanosheets and the metal nanoparticles. The heterogeneous Mott–Schottky catalyst can be reused for five cycles without any obvious loss of its catalytic activity.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Jianfeng Shan,Zheng Chen,Dengfeng Wang,Guangyu Zhang,Sheng Li,Chuan Sun,Dongchao Wang,Caixia Ju,Xuelan Zhang,Lei Li
Catalytic conversion of ethyl levulinate (EL) to γ-valerolactone (GVL) is a pivotal reaction in biomass conversion. Here, Pd/CoO x was studied and showed much higher EL hydrogenation reactivity than other Pd based catalysts. Further investigation revealed that EL conversion increased linearly with PdCo alloying degree elevating, indicating that PdCo alloy is ascribed to the superior reactivity of Pd/CoO x . Interestingly, Pd/CoO x with low Pd loading also exhibited excellent hydrogenation performance, and surface enrichment of Pd was identified as the main reason. Additionally, employing HZSM-5 as a co-catalyst not only accelerated ethyl 4-hydroxypentanoate lactonization, but also dramatically improved the stability of Pd/CoO x . As a result, a 99.1 % yield of GVL was achieved by the synergistic catalysis of HZSM-5 and Pd/CoO x containing 0.58 wt% Pd, which is comparable with the best catalyst ever reported in alkyl levulinate hydrogenation to GVL. Furthermore, the insights gained from this work have broad potential applications in biomass hydrogenation.
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MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 12
·1-10
·
IF 5.3
Li Chengcheng,Lu Jinhui,Xiang Chao,Zhang Enhui,Tian Xiaofang,Zhang Ling,Li Tingting,Li Chengyao
Three-metal-core-shell nanoparticles (Au@Pt@PdNPs) providing excellent peroxidase-like activity were applied in lateral flow immunoassay (LFIA), designated as Au@Pt@Pd-LFIA, for detecting the nucleocapsid protein (NP) of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2). An Au@Pt@Pd-LFIA was developed for quantitatively testing of SARS-CoV-2 NP with a range 0.12–31.25 ng/mL. The limit of detection (LOD) of Au@Pt@Pd-LFIA strip was 0.06 ng/mL, which was 16-fold or eightfold more sensitive than that of the gold lateral flow immunoassay (Au-LFIA) and the gold flower flow immunoassay (AF-LFIA) strips, respectively. For detection of clinical samples from nasal swabs using test strips, Au@Pt@Pd-LFIA had 84.09% sensitivity, 100% specificity, and 92.55% accuracy. In terms of detection time, the testing of Au@Pt@Pd-LFIA strip was 16 min similar to Au-LFIA (15 min) and AF-LFIA (10 min), but much shorter than ELISA (2 h). In conclusion, Au@Pt@Pd-LFIA is a sensitive, rapid, and simple test for quantitative detection of SARS-CoV-2 NP in nasal swab samples. Graphical Abstract
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FUEL
·
2024
·
IF 6.7
Yang Sun,Fan Yang,Siyuan Sun,Yankun Sun,Hongchen Liu,Chunhui Yu,Junpu An,Xi Li,Yongfeng Li
The preparation of highly active and stable Pd-based catalysts for direct alcohol fuel cells (DAFC) is hampered by inefficient utilization of the active sites, susceptibility to CO poisoning, poor stability, and relatively slow reaction kinetics. Herein, the stability and anti-toxicity of the catalysts (Pd/ZnO/MDC) are tuned by loading Pd nanoparticles on the carbon-coated ZnO support, achieving efficient electrocatalysis for methanol and ethanol oxidation reaction (MOR and EOR). TEM result shows the ZnO is covered by the carbon layer formed outside of MOF-5 derived porous carbon, which can prevent it from dissolving under harsh conditions. The mass activities of the well-tuned catalyst Pd/ZnO/MDC (8 0 0) for MOR and EOR are 931.83 mA/mg and 1838.30 mA/mg, respectively. It is due to the improved electron transport efficiency between the Pd and ZnO, and the enhanced stability by carbon layer outside the ZnO. It is also found that the onset potential and the peak potential of Pd/ZnO/MDC (8 0 0) (−0.813 V, −0.228 V) in CO stripping experiment in MOR are more negative than Pd/MDC (8 0 0) (−0.261 V, −0.215 V). This result indicates that the existence of ZnO helps to provide surface hydroxyl group, which promotes the oxidation of the intermediates. This work indicates provides a feasible idea for DAFC catalyst design and construction.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2016
·
IF 3.205
Yuan-Hang Qin,Zi-Yao Xiong,Jiayu Ma,Li Yang,Zaikun Wu,Weiliang Feng,Tie-Lin Wang,Wei-Guo Wang,Cun-Wen Wang
TiO 2 -modified nitrogen-doped carbon (TiO 2 -NC), prepared by a polymerization-pyrolysis process, is used to support the Pd catalyst for ethanol oxidation reaction (EOR) in alkaline media . X-ray photoelectron spectroscopy characterization indicates that the incorporation of TiO 2 and nitrogen into the carbon matrix could improve the percentage of Pd 0 in Pd/TiO 2 -NC catalyst. Electrochemical characterization shows that the Pd/TiO 2 -NC catalyst presents higher electrocatalytic activity and stability for EOR than the nitrogen-doped carbon-supported Pd (Pd/NC) catalyst and the carbon black-supported Pd (Pd/CB) catalyst, which can be mainly attributed to the high percentage of Pd 0 in Pd/TiO 2 -NC catalyst (65%) than those in Pd/NC (48%) and Pd/CB (31%) catalysts. The results indicate that the Pd/TiO 2 -NC catalyst holds great potential as high-performance anode catalyst for direct ethanol fuel cells.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2016
·
IF 8.328
Jiawei Xia,Yongsheng Fu,Guangyu He,Xiaoqiang Sun,Xin Wang
A magnetically separable core-shell-like catalyst Ni-Pd/CB is designed and synthesized via a facile sequential reduction strategy. It is found that the Pd nanocrystals with a thickness of ∼1.67 nm and a length of ∼7.92 nm are intimately coupled with the Ni cores and the formed core-shell-like Ni-Pd nanoparticles are well dispersed on the CB surface with much smaller particle size and narrower size distribution as compared with that of unsupported ones. The ligand-free Ni-Pd/CB nanocatalyst is evaluated for Suzuki-Miyaura coupling reaction and exhibits excellent catalytic activity under mild aerobic conditions without using toxic solvents and inert protective atmosphere, achieving green catalysis. The high catalytic performance of Ni-Pd/CB catalyst can be attributed to its unique core-shell-like nanostructure and the concerted effects between the individual components. The introduction of Ni not only makes the catalyst magnetically separable in a suspension system, but also significantly lowers the cost.
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BIOSENSORS & BIOELECTRONICS
·
2015
·
IF 6.409
Yicheng Wei,Yan Li,Na Li,Yong Zhang,Tao Yan,Hongmin Ma,Qin Wei
In the present work, an ultrasensitive sandwich-type electrochemical immunosensor based on a novel signal amplification strategy was designed for quantitative detection of alpha fetoprotein (AFP). Au nanoparticles with biocompatibility were electrodeposited on the surface of glassy carbon electrode (GCE) which can effectively capture and immobilize primary anti-AFP (Ab 1 ) to significantly amplify the electrochemical signal. Graphene Oxide and CeO 2 mesoporous nanocomposite functionalized by the 3-aminopropyltriethoxysilane supported Pd octahedral nanoparticles (Pd/APTES-M-CeO 2 -GS) were utilized as labels of detection anti-AFP (Ab 2 ). Pd octahedral nanoparticles presented good catalytic activity towards the reduction of H 2 O 2 . Due to the large specific surface area and good adsorption properties of APTES-CeO 2 -GS nanocomposite, large amount of Pd octahedral nanoparticles could be immobilized, which could amplify the electrochemical signal and improve the sensitivity of the immunosensor. Under optimal conditions, the immunosensor exhibited wide linear range from 0.1 pg/mL to 50 ng/mL with a low detection limit of 0.033 pg/mL ( S / N =3) for AFP detection. In addition, high sensitivity, excellent selectivity, good reproducibility and stability were obtained for the immunosensor, which has a promising application for quantitative detection of other tumor markers in clinical diagnosis.
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ACS Applied Materials & Interfaces
·
2016
·
IF 7.145
Shu-He Han,Juan Bai,Hui-Min Liu,Jing-Hui Zeng,Jia-Xing Jiang,Yu Chen,Jong-Min Lee
Noble metal nanostructures (NMNSs) play a crucial role in many heterogeneous catalytic reactions. Hollow and porous NMNSs possess generally prominent advantages over their solid counterparts due to their unordinary structural features. In this work, we describe a facial one-pot synthesis of hollow and porous Pd–Cu alloy nanospheres (Pd–Cu HPANSs) through a polyethylenimine (PEI)-assisted oxidation–dissolution mechanism. The strong coordination interaction between CuII and PEI facilitates the oxidation–dissolution of the Cu2O nanospheres template under air conditions, which is responsible for the generation of the Pd–Cu alloy and the convenient removal of the Cu2O nanospheres template at room temperature. Compared to the commercial Pd black, the Pd–Cu HPANSs show remarkably improved catalytic activity for the reduction of K2Cr2O7 by HCOOH at room temperature, attributing to the enhanced catalytic activity of the Pd–Cu HPANSs for the dehydrogenation decomposition of HCOOH.
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危险品化学品经营许可证（带存储）