CHINESE JOURNAL OF ANALYTICAL CHEMISTRY
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2021
·
IF 1.134
Yan-Xiong LIU,Long-Chun BIAN,Jie-Ren XIA,Qiu-E CAO
A novel Pd(II) ion-imprinted polymer (Pd(II)-AAP-IIP@VMWCNTs) was constructed by using 2-( N -allyl)aminopyridine (AAP), vinyl functionalized multi-walled carbon nanotubes (VMWCNTs), ethylene glycol dimethacrylate (EGDMA) and Na 2 PdCl 4 as functional monomer, carrier, cross-linker and template ions, respectively. The structure, morphology, adsorption property and applicability as adsorbent in solid phase extraction were characterized by Fourier transform infrared (FTIR) spectroscopy, transmission electron microscopy (TEM), scanning electron microscopy (SEM), binding experiment and solid phase extraction (SPE) experiment, respectively. The equilibrium adsorption capacity and imprinting factor of Pd(II)-AAP-IIP@VMWCNTs for Pd(II) were found to be 9.053 mg/g and 3.46, respectively. The SPE column packed with Pd(II)-AAP-IIP@VMWCNTs displayed good adsorption selectivity to Pd(II). The adsorption rate and extraction rate of this column to Pd(II) were more than 90% and 74%, but below 40% and 15% to the other coexisting ions under the optimized SPE conditions. The obtained Pd(II)-AAP- IIP@VMWCNTs-based SPE method could be combined with inductively coupled plasma optical emission spectroscopy (ICP-OES) for determination of Pd(II) in environmental water. The recoveries were in the range of 87.2%–91.6% with the relative standard deviations of 2.5%–6.8%.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2021
·Vol. 29
·期 2
·1824-1835
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IF 4.223
Chen Yuan,Chen Yuancai
At present, there are many studies on microbial reduction of Pd (II), although few of these studies assess the bacterial toxicity of Pd (II) before and after reduction by microorganisms. In this study, the toxicity of Pd (II) to Bacillus wiedmannii MSM ( B. wiedmannii MSM) was assessed before and after reduction by live B. wiedmannii MSM cells (referred to as “Pd (0)-loaded cells”) and after biosorption by dead B. wiedmannii MSM cells (referred to as “Pd (II)-loaded cells”). B. wiedmannii MSM is a widely occurring, nonpathogenic aerobic bacterium. Compared with Pd (II), the EC 20 , EC 50 , and EC 80 of Pd (0)-loaded cells increased by 77.73-, 112.75-, and 163.91-fold, respectively, while the EC 20 , EC 50 , and EC 80 of Pd (II)-loaded cells increased by only 11.55-, 9.77-, and 8.29-fold, respectively. The sterilization contribution rates of the mechanisms of action of Pd (0)-loaded cells were ranked in the order of: remaining Pd (II) > oxidative stress > physical puncture. Pd (II) was found to increase cell membrane permeability, glutathione S-transferase (GST) enzyme activity, and reactive oxygen species levels in cells and decrease the cell membrane potential. XPS results indicated that Pd (II) increased the content of polysaccharides and peptides and decreased the content of hydrocarbons in cells. These findings reveal the bactericidal mechanism of toxicity of Pd (II) and Pd (0)-loaded cells on Bacillus wiedmannii MSM and provide an environmentally friendly and inexpensive method for Pd (II) detoxification.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Xiaoli Li,Ting Wang,Ziqiang Zheng,Qing Yang,Can Li,Benxia Li
Developing photocatalysts for coproduction of hydrogen fuel and valuable chemicals is highly desired but still challenging. Herein, Pd-modified defective HNb 3 O 8 photocatalyst (denote as Pd/HNb 3 O 8 -H 2 ) consisting of dispersive Pd sites and abundant surface oxygen vacancies (V O s) was prepared via the thermal treatment of Pd 2+ -incorporated HNb 3 O 8 in H 2 /Ar gas. The existence of Pd favors the formation of V O s on HNb 3 O 8 , enabling the synchronous construction of Pd and V O dual active sites. The spectroscopy and photoelectrochemical studies demonstrate the advantages of Pd/HNb 3 O 8 -H 2 photocatalyst in promoting the separation and migration of photoinduced charge carries. The Pd/HNb 3 O 8 -H 2 photocatalyst exhibits the outstanding performance toward photocatalytic proton reduction coupled with selective benzyl-alcohol oxidation , achieving the optimal production rates of H 2 and benzaldehyde as high as 3.17 and 2.76 mmol·g cat −1 h −1 , respectively. The experimental and theoretical investigations have expounded the synergistic mechanism of Pd and V O dual active sites in boosting photocatalytic coproduction of H 2 and benzaldehyde.
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Catalysts
·
2021
·Vol. 11
·期 8
·888
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IF 4.146
Jingzhen Wang,Kaijie Mu,Xuedong Zhao,Dianliang Luo,Xiaodi Yu,Wenpeng Li,Jie Chu,Jing Yang,Qinzheng Yang
Metal, as a high-performance electrode catalyst, is a research hotspot in the construction of a high-performance microbial fuel cell (MFC). However, metal catalyst nanoparticles and their dispersed carriers are prone to aggregation, producing catalytic electrodes with inferior qualities. In this study, Pd is uniformly dispersed on the graphene framework supported by carbon black to form nanocomposite catalysts (Pd/GO-C catalysts). The effect of the palladium loading amount in the catalyst on the catalytic performance of the air cathode was further studied. The optimized metal loading afforded a reduced resistance and improved accessibility of Pd particles for the ORR. The maximum current output of the 0.250 Pd (mg/cm2) MFC was 1645 mA/m2, which is 4.2-fold higher than that of the carbon paper cathode. Overall, our findings provide a novel protocol for the preparation of high-efficient ORR catalyst for MFCs.Keywords:oxygen reduction reaction;microbial fuel cell;air cathode
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NEOPLASIA
·
2021
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IF 5.715
Yihui Ma,Peiyi Xia,Zhengyang Wang,Jingjing Xu,Lan Zhang,Yanan Jiang
Protein Disulfide Isomerase Family A Member 6 (PDIA6) is an endoplasmic reticulum protein that is capable of catalyzing protein folding and disulfide bond formation. Abnormally elevated expression of PDIA6 has been reported to predict poor outcomes in various cancers. Herein, gain-of- and loss-of-function experiments were performed to investigate how PDIA6 participated in the carcinogenesis of pancreatic cancer (PC). By analyzing the protein expression of PDIA6 in 28 paired PC and para carcinoma specimens, we first found that PDIA6 expression was higher in PC samples. Both the overall survival and disease-free survival rates of PC patients with higher PDIA6 expression were poorer than those with lower PDIA6 ( n = 178). Furthermore, knockdown of PDIA6 impaired the malignancies of PC cells — suppressed cell proliferation, invasion, migration, cisplatin resistance, and xenografted tumor growth. PDIA6-silenced PC cells were more sensitive to cytotoxic natural killer (NK) cells. Overexpression of PDIA6 had opposite effects on PC cells. Interestingly, COP9 signalosome subunit 5 (CSN5), a regulator of E3 ubiquitin ligases known to promote deubiquitination of its downstream targets, was demonstrated to interact with PDIA6, and its expression was increased in PC cells overexpressing PDIA6. Additionally, PDIA6 overexpression promoted deubiquitination of β-catenin and PD-L1 and subsequently upregulated their expression in PC cells. These alterations were partly reversed by CSN5 shRNA. Collectively, the above results demonstrate that PDIA6 contributes to PC progression, which may be associated with CSN5-regulated deubiquitination of β-catenin and PD-L1. Our findings suggest PDIA6 as a potential target for the treatment of PC.
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ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Hao Huang,Rui Zong,Hao Li
This work reports an innovative route for biomass upgrading via hydrodeoxygenation (HDO) reactions which avoids external high-pressure hydrogen supply and harsh conditions (such as high-temperature or additives). A novel Pd/CFR catalyst with controllable oxygen groups and defects was synthesized with low-load Pd supported on resorcinol–formaldehyde resin carbon spheres (CFR) for selective hydrodeoxygenation of vanillin under mild conditions. The as-prepared Pd/CFR-800 catalyst shows excellent activity (>99.5% yield of 2-methoxy-4-methylphenol) using polymethylhydrosiloxane (PMHS) as green hydride source within 1 h at 70 °C, in the absence of additives. According to spectral analyses, the concentration of carbon skeleton defects and hydroxyl functional groups on the catalyst can be adjusted by the carbonization temperature. Combined with experimental results and mechanistic studies, the synergistic effect of hydroxyl groups and adjacent defects was deemed as the main reason for the strong adsorption of the substrate, which significantly facilitated the key hydrogenolysis step. Furthermore, the as-prepared Pd/CFR-800 catalyst has shown excellent recyclability after used for five times. The in situ regulation of functional groups and defects on carbon materials provides new ideas for designing high-performance catalysts for the catalytic transformation of various lignin derivatives.
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Molecular Catalysis
·
2020
·
IF 3.687
Qian Wang,Meiling Ge,Yuheng Dou,Fu Yang,Junkai Wang,Yuyang Shao,Agen Huang
Polymer supports play an important role in noble metal loaded catalysts. In this study, palladium clusters stabilized by several polyamides have been widely studied in the oxidation of benzyl alcohol under airflow. The different kinds of polyamides (PADs) were synthesized with aromatic diamines and trimesoyl chloride by mechanical grinding method and solvent-heat method. Polyamide support was synthesized through mechanical grinding method. And the laminar structure and abundant amide bonds of polyamide can help obtain ultrafine Pd clusters with a mean particle size of 1.76 nm. The Pd 0.5 @PAD-2-M effectively catalyzed benzyl alcohol into benzaldehyde with a conversion of 96.1 % and turnover number (TON) of 1441 under 90 °C in water which was 2.5 times higher than the commercial Pd/C catalyst. High TON value of 6505 was also achieved in solvent-free system. This work reveals the advantages of laminar structure of polyamide in dispersing Pd clusters and promoting benzyl alcohol conversion. Besides, the carrier properties of amphipathy and substrate adsorption were also investigated to illustrate the significance of interfacial effect for laminar catalyst in heterogeneous catalysis.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
·
IF 8.128
Xingchi Li,Huaming You,Cheng Wang,Dongmei Liu,Rui Yu,Siyu Guo,Yuan Wang,Yukou Du
Modifying the electronic structure and optimizing the geometric structure can expeditiously tune the electrocatalytic properties of catalysts, resulting in considerably enhanced electrocatalytic performance towards electrocatalytic oxidation of liquid fuels . We herein report a simple synthetic strategy to prepare Bi-doped 3D taraxacum-like Pd nanocages (NCs) composed of porous nanosheets , which possess high surface areas and strong synergistic effects. Notably, a trace of Bi diffuses into the lattice of Pd and increases the electronic effects of the surface of Pd, endowing PdBi-0.5 NCs/C with superior electrocatalytic performance towards ethanol oxidation reaction (EOR). The mass activity and specific activity of PdBi-0.5 NCs/C were 3494.8 mA mg Pd −1 and 10.37 mA cm −2 , being 4.08- and 4.82- fold enhancements as compared with commercial Pd/C, respectively. Moreover, the highly open porous 3D nanocages structure with rich active sites and defects can also facilitate the mass/electron transfer to favor the EOR kinetics.
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ACS Catalysis
·
2020
·
IF 12.35
Zhongjie Cai,Jiajun Dai,Wen Li,Kok Bing Tan,Zhongliang Huang,Guowu Zhan,Jiale Huang,Qingbiao Li
Utilization of CO2 and its conversion to value-added chemicals are highly desirable to alleviate the environmental concerns caused by the massive anthropogenic CO2 emission. Although In2O3/Pd have been employed as efficient catalysts for hydrogenation of CO2 to methanol, the electronic effects by strong metal–support interaction (SMSI) between Pd and In2O3 are poorly understood, which is greatly affected by the morphology of In2O3. Herein, we use MIL-68(In) nanorod as a morphological template for the synthesis of hollow In2O3 nanotubes (h-In2O3) and the preparation of supported Pd catalysts for CO2 hydrogenation to methanol. Interestingly, loading Pd on h-In2O3 showed a much higher performance than In2O3 with other morphologies, which exhibited almost unchanged CO2 conversion of 10.5%, methanol selectively of 72.4%, and methanol space-time yield of 0.53 gMeOH h–1 gcat–1 over 100 h on stream at 3 MPa and 295 °C. After in-depth characterizations, we found that the different electronic properties of Pd species on In2O3 can be finely tuned by diverse synthetic conditions, which were responsible for high activity and stability. The molar fraction of Pd2+ species in the h-In2O3/Pd catalyst reached 67.6%, 3.2 times that of the In2O3@Pd catalyst (21.3%), due to the different surface chemistry of In2O3. Density function theory results indicated that the Pd donated more electrons to the curved In2O3 (222) surface than the pristine surface, and Pd2+ was critical to facilitate H2 adsorption and formation of the surface oxygen vacancy. This work demonstrates that controlling the morphology of In2O3 can modify both the Pd electronic property and SMSI between Pd and In2O3, which are the origins of the high catalytic performance.
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Nanoscale
·
2020
·Vol. 13
·期 6
·3528-3542
·
IF 6.895
Yaxing Liu,Weiyin Li,Guizhe Zhao,Gang Qin,Yuexia Li,Yaqing Liu
The lack of direct insight into the microstructural evolution of catalytic materials under electrochemical polarization has inhibited the development of heterogeneous catalysts. By investigating a typical Au@Pd core–shell nanostructure, the present study discloses the microstructural evolution of heterogeneous catalytic materials during the methanol electrooxidation reaction (MOR). The electrocatalytic activity of the as-prepared Au@Pd_core–shell nanoparticles continuously increased during the first 100 successive voltammetry cycles of the MOR. Microstructural characterization studies revealed that during the MOR, an Au/Pd mixed bimetallic shell was formed by the self-driven microstructural evolution of the Au@Pd_core–shell nanoparticles. Both the experimental and calculation results indicated that the Au/Pd mixed bimetallic shell reduced the binding strength of OH− and CO on the catalyst surface. The exposed Au atoms in the shell region also produced large-scale reactive ˙OH radicals that facilitated the oxidative removal of the adsorbed carbonaceous species from the adjacent Pd active sites.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Jiasheng Zhou,Zimo Lou,Zheni Wang,Chuchen Zhou,Cheng Li,Shams Ali Baig,Xinhua Xu
The CTAB-Pd/GAC catalyst was obtained by functionalizing palladium/granular activated carbon (Pd/GAC) with cetyltrimethylammonium bromide (CTAB), which was used for the electrocatalytic reductive dechlorination of 2,4-dichlorobenzoic acid (2,4-DCBA). The degradation rate of 2,4-DCBA by 40 mg g −1 CTAB-Pd/GAC was 9.8 × 10 −3 (min −1 g −1 Pd), which was 11 folds than that by Pd/GAC (0.9 × 10 −3 min −1 g −1 Pd), and the value of q e, 2,4-DCBA / q e, BA was 2.33 as compared to 0.67 for Pd/GAC. The combined result of dechlorination and adsorption experiments suggested that the functionalization by CTAB would enhance the 2,4-DCBA concentration on the surface of CTAB-Pd/GAC, and accelerate the degradation rate. However, the removal efficiency of 2,4-DCBA would decrease when the CTAB load reached 80 mg g −1 , due to the excessive adsorption capacity for dechlorinated product. Density functional theory (DFT) calculations also proved that CTAB would increase adsorption capacity of catalyst and selective adsorption behavior of 2,4-DCBA, which accelerated the degradation rate of 2,4-DCBA.
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2020
·Vol. 36
·期 5
·934-939
·
IF 1.063
Li Ruyue,Wu Mingwei,Pan Biwei,Li Meng,Huang Jun
A 1,10-phenanthroline based polymer named PPPhen( i.e. , polymer from pyrene 1,10-phenanthrolin) was prepared by the Friedel-Crafts reaction of 1,10-phenanthroline and pyrene cross-linked with dimethoxymethane. The related Pd catalyst Pd@PPPhen was prepared by supporting Pd nanoparticles(NPs) on the PPPhen material. PPPhen and Pd@PPPhen were characterized by means of scanning electron microscopy(SEM), transmission electron microscopy, N 2 adsorption-desorption, Fourier-transform infrared and X-ray photoelectron spectroscopy analyses. The results showed that PPPhen polymer was highly porous and that the phenanthroline group can enhance the stability of the Pd nanoparticles. Pd@PPPhen also exhibited good catalytic activity in the aerobic oxidation of alcohols to aldehydes and ketones, and Pd@PPPhen was recyclable with durable activity and retentive structures.
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