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Gels · 2023 ·Vol. 9 ·期 1 ·64 · IF 4.6

Facile Synthesis and Fabrication of NIPAM-Based Cryogels for Environmental Remediation

Jaweria Ambreen,Abdul Haleem,Aqeel Ahmed Shah,Fozia Mushtaq,Muhammad Siddiq,Muhammad Ali Bhatti,Syed Nizam Uddin Shah Bukhari,Ali Dad Chandio,Wael A. Mahdi,Sultan Alshehri

Herein, polymeric cryogels containing poly(N-isopropylacrylamide) were synthesized by cryo-polymerization at subzero temperature. The synthesized cryogels were loaded with silver and palladium nanoparticles by the chemical reduction method at room temperature using the reducing agent NaBH4. Moreover, for comparison with cryogels, pure poly(N-isopropylacrylamide) hydrogel and its silver hybrid were also prepared by the conventional method at room temperature. The chemical structure and functional group analysis of the pure cryogels was confirmed by Fourier transform infrared spectroscopy. The synthesis of hybrid cryogels was confirmed by the X-ray diffraction technique and energy dispersive X-ray. The pore size and surface morphology of the pure cryogels, their respective hybrid cryogels and of conventional hydrogels were studied by using the scanning electron microscopy technique. The hybrid cryogels were successfully used as a catalyst for the degradation of methyl orange dye. The degradation performance of the hybrid cryogels was much better than its counterpart hybrid hydrogel for methyl orange dye. The effect of temperature and amount of catalyst on catalytic performance was studied by UV-visible spectroscopy. The reduction follows pseudo-first-order reaction kinetics. In addition, the antibacterial activities of these cryogels were evaluated against Gram-positive bacteria (Staphylococcus aureus, ATCC: 2593) and Gram-negative bacteria (Escherichia coli, ATCC: 25922). Both hybrid cryogels have shown much better antibacterial activity for these two strains of bacteria compared to pure cryogels. The results indicate that these cryogels are potential candidates for water purification systems as well as biomedical applications.

研究领域: 环境科学 · 材料科学 · 生物医学
✓ 已验证 DOI 高影响因子
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RSC Advances · 2019 ·Vol. 9 ·期 21 ·12134-12145 · IF 3.049

Hybrid ZnO–graphene electrode with palladium nanoparticles on Ni foam and application to self-powered nonenzymatic glucose sensing

Wenyi Wu,Fengjuan Miao,Bairui Tao,Yu Zang,Lei Zhu,Cuiping Shi,Paul K. Chu

A self-powered nonenzymatic glucose sensor electrode boasts the advantages of both a glucose sensor and fuel cell. Herein, an electrode composed of ZnO–graphene hybrid materials on nickel foam (NF) is prepared by electrodeposition of Pd NPs. The electrode is characterized systematically and the dependence of electrocatalytic oxidation of glucose on the concentrations of KOH and glucose, temperature, and potential limit in the anodic direction is investigated. The Pd/NF-ZnO–G electrode shows high catalytic activity, sensitivity, stability, and selectivity in glucose detection, as exemplified by an electrocatalytic glucose oxidation current of 222.2 mA cm−2 under alkaline conditions, high linearity in the glucose concentration range from 5 μM to 6 mM (R2 = 0.98), and high sensitivity of 129.44 μA mM−1−1 cm−2. The Pd/NF-ZnO–G electrode which exhibits superior electrocatalytic activity under alkaline conditions has large potential in nonenzymatic glucose sensing and direct glucose fuel cells and is suitable for miniaturized self-powered nonenzymatic glucose sensing.

研究领域: 生物医学工程 · 材料科学 · 分析化学
✓ 已验证 DOI 高影响因子
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Catalysis Science & Technology · 2021 ·Vol. 11 ·期 13 ·4398-4405 · IF 6.119

Size-dependent strong metal–support interaction in Pd/ZnO catalysts for hydrogenation of CO2 to methanol

Liangcai Zhang,Xinyu Liu,Hengwei Wang,Lina Cao,Chenxi Huang,Shang Li,Xiaohui Zhang,Qiaoqiao Guan,Xiang Shao,Junling Lu

Strong metal–support interaction (SMSI) has long been studied in catalytic reactions. Proper utilization of the SMSI effect might not only improve the stability of the catalysts, but also the activity and selectivity. In this work, using the atomic layer deposition (ALD) technique, we synthesized a series of Pd/ZnO catalysts with Pd particle sizes ranging from 1.6 to 7.9 nm. Upon H2 reduction at elevated temperatures, these Pd/ZnO catalysts display a size-dependent SMSI effect wherein the larger-size Pd particles are more prone to be encapsulated by ZnO compared to the smaller ones. In the reaction of CO2 hydrogenation, we show that such size-dependent SMSI, together with the size-related CO binding strength on Pd particles, provides a higher activity and methanol selectivity to the Pd particles larger than ~2.5 nm.

研究领域: 催化化学 · 材料科学
✓ 已验证 DOI 高影响因子
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FUEL · 2021 · IF 6.609

Hydrodeoxygenation of vanillin to creosol under mild conditions over carbon nanospheres supported palladium catalysts: Influence of the carbon defects on surface of catalysts

Tong Li,Hao Li,Chunli Li

Hydrodeoxygenation (HDO) is a promising process for biomass upgrading. A challenge is designing and developing related efficient catalysts. Here, we developed a defects enhancement engineering to synthesize carbon-based supported Pd catalysts (0.5%Pd/CNS) for vanillin HDO under mild condition. It is found that the degree of carbon defects was negative correlation with the cross-linked degree of resorcinol–formaldehyde (RF) resin sphere (carbon precursor), which can be modulated by amount of ammonium fluoride (NH 4 F) (0, 0.01, 0.03, and 0.05 g). The RF resin sphere (RF-0.03) with the lowest cross-linked degree was obtained by addition of 0.03 g NH 4 F, and then 0.5%Pd/CNS-0.03 possessed rich carbon defects obtained by carbonization of RF-0.03. The catalyst possessing the most degree of carbon defects (1.96 of A D1 /A G from Raman data, D1 ∼ defective carbon, G ∼ graphitic carbon) exhibited the highest activity among as-prepared catalysts: 100% of vanillin conversion and 100% of yield to creosol in vanillin HDO over 0.5%Pd/CNS-0.03 (0.03 g of NH 4 F) at 60 °C, 0.1 MPa H 2 , and 1 h. The excellent performance can be attributed to the rich carbon defects on surface of catalysts, which can play an important role on growth of active metal and activation of reactants. This work improves green catalysis of HDO with a strategy of defect engineering to surface microenvironment modulation.

研究领域: 催化 · 绿色化学 · 生物质升级 · 材料科学
✓ 已验证 DOI 高影响因子
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JOURNAL OF SUPERCRITICAL FLUIDS · 2015 · IF 2.371

Mesoporous spherical silica encapsulating Pd nanoparticles prepared by CO2-induced mircoemulsion and catalytic application in Suzuki coupling reaction

Li Guo,Xiuge Zhao,Ran Zhang,Chen Chen,Jizhong Chen,Angjun Chen,Xuerui Liu,Zhenshan Hou

The CO 2 -in-water (C/W) microemulsion was formed when the pressure of CO 2 was above 4.0   MPa and has been investigated in-situ via high-pressure UV/vis spectra. The spherical mesoporous silica was successfully synthesized in CO 2 -induced microemulsion. Uniform spherical silica with a diameter of 102   ±   15   nm can be obtained by using C/W microemulsion as a template. It was observed that the BET area and pore volume of the spherical silica were enlarged with increasing the pressure of CO 2 . Moreover, Pd nanoparticles (Pd NPs) were encapsulated inside the spherical mesoporous silica through one-pot approach. Owing to the particular core–shell structure, this catalyst showed excellent recyclability in the Suzuki coupling reaction when compared with conventional Pd/SiO 2 and Pd/C catalysts. The new strategy can be extended as a general approach to prepare other metal nanoparticles encapsulated in spherical mesoporous silica.

研究领域: 材料科学 · 化学工程 · 催化技术
✓ 已验证 DOI 高影响因子
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MICROPOROUS AND MESOPOROUS MATERIALS · 2021 · IF 5.455

Hydrogen accelerated regeneration of FeII in Fenton reaction enhanced by Pd/MOF-808(Zr)

Yang Hu,Hai-Liang Yang,San-Jian Ma,Juan-Hong Li,Xin Liu,Yong-Jing Tian,Long Jin,Zi-Xia Lin

The promotion of Fenton process in organic wastewater treatment has been hindered by the disposal of large amounts of iron sludge derived from the excess addition of ferrous salt. The operation of the Fenton reaction could be maintained using trace level Fe II through the effective acceleration reaction of active hydrogen. However, the H 2 which is the precursor of active hydrogen is insoluble in water. Herein, the composite catalyst Pd/MOF-808(Zr) was introduced into the H 2 -Fenton system to enhance the adsorption and activation of this reducing gas. In this novel improved Fenton system called MHACF-MOF-808(Zr), the hydroxyl radical would be unceasingly produced based on the unceasingly recycling of FeII/FeIII at normal temperature and pressure. 15 mg L −1 sulfamethazine could be thoroughly degraded during 2 h reaction process in the initial condition of 60 mL min −1 H 2 , 20 μmol L −1 Fe II , pH 3, 20 mmol L −1  H 2 O 2 and 2 g L −1  Pd/MOF-808(Zr). And so did 10 mg L −1 2,4-Dichlorophenol. The activity and stability of Pd/MOF-808(Zr) could be maintained after at least 6 consecutive reaction cycles. It provides new insight for improving the inherent shortcoming of the Fenton reaction which will generate large amounts of iron sludge.

研究领域: 环境科学 · 化学工程
✓ 已验证 DOI 高影响因子
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Journal of Materials Chemistry A · 2015 ·Vol. 3 ·期 46 ·23230-23239 · IF 7.443

Polymer-templated synthesis of hollow Pd–CeO2 nanocomposite spheres and their catalytic activity and thermal stability

Chenhao Du,Yun Guo,Yanglong Guo,Xue-qing Gong,Guanzhong Lu

Developing methods for the fabrication of active and thermally stable noble metal/metal oxide nanomaterials are very important for catalysis and material fields. Herein, we used a polymer-template synthesis approach to prepare hollow Pd–CeO2 nanocomposite spheres (NCSs) with Pd nanoparticles evenly distributed inside the CeO2 shell, in which the aggregation of Pd nanoparticles can be well inhibited with the help of the protection of CeO2 nanocrystallites even after being calcined at 700 °C. The Pd nanoparticles are partially buried in the CeO2 shell and the surface Pd species are highly ionic, which is caused by the electron exchange at the Pd–CeO2 interface during calcination. This hollow structure Pd–CeO2 nanocatalyst shows excellent catalytic activity and stability in the aqueous selective reduction of 4-nitrophenol and gaseous CO oxidation. For the selective reduction of 4-nitrophenol, the reaction rate of this h-Pd–CeO2 NCS catalyst compared to those of the supported Pd/CeO2 and physically mixed Pd + CeO2 catalysts is almost 14 times and 5 times faster, respectively. For the CO oxidation, the larger Pd–CeO2 interface in h-Pd–CeO2 NCSs could facilitate the reaction between the adsorbed CO and O2, thus showing better low temperature activity. This paper emphasizes the advantages of a core–shell hollow structure and provides a new way for obtaining novel functional nanocatalysts.

研究领域: 材料化学 · 纳米催化 · 无机功能材料 · 环境催化 · 能源材料
✓ 已验证 DOI 高影响因子
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DALTON TRANSACTIONS · 2015 ·Vol. 44 ·期 31 ·13906-13913 · IF 4.197

Controlled synthesis of uniform palladium nanoparticles on novel micro-porous carbon as a recyclable heterogeneous catalyst for the Heck reaction

Kunpeng Song,Peng Liu,Jingyu Wang,Lei Pang,Jian Chen,Irshad Hussain,Bien Tan,Tao Li

Novel dual-porous carbon-supported palladium nanoparticle (Pd NP) catalysts were prepared by sequential carbonization and reduction of microporous organic polymer-encaged PdCl2. The diverse pore structure of microporous organic polymers provides a reservoir for the palladium precursors and prevents Pd NPs from sintering during the carbonization and reaction. The microporous structure has a significant effect on the size and dispersion of palladium NPs. The average size of the Pd NPs (in the range of 4–6 nm) was tuned by changing the pore size distribution and the carbonization temperature. The resulting carbon-supported Pd NPs were characterized by TEM, BET, XRD, and XPS and the Pd loading was calculated by AAS. The encaged Pd NP catalysts prepared by this methodology exhibited outstanding stability and reusability in the Heck reaction and could be reused at least 10 times without appreciable loss of activity.

研究领域: 材料化学 · 纳米催化 · 有机合成方法学 · 多孔材料 · 绿色化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF POLYMER SCIENCE PART A-POLYMER CHEMISTRY · 2015 ·Vol. 53 ·期 12 ·1457-1463 · IF 3.113

Investigation of Suzuki–Miyaura catalyst-transfer polycondensation of AB-type fluorene monomer using coordination-saturated aryl Pd(II) halide complexes as initiators

Zilong Zhang,Pan Hu,Xiao Li,Hongmei Zhan,Yanxiang Cheng

Novel triarylamine-based coordination-saturated aryl Pd(II) halide complexes ligated by PEt 3 , PCy 3 , and P( o -tol) 3 were successfully synthesized by direct oxidative addition of aryl halide to the corresponding Pd(0) precursors. Suzuki–Miyaura coupling polymerization of 2-(7-halide-9,9-dioctylfluoren-2-yl)−1,3,2-dioxaborinane with these Pd(II) complexes as initiators was investigated for the synthesis of poly(fluorene)s with triarylamine end group. Pd(II) complexes with PCy 3 or P( o -tol) 3 exhibited catalytic activity and realized the catalyst-transfer polycondensation at 75 °C and room temperature, respectively, while the polymerization using Pd(II) catalyst ligated by PEt 3 did not proceed, which indicated that the bulky phosphine ligands could facilitate the reductive elimination and further promote the polymerization. In addition, the dimeric Pd(II) complex with P( o -tol) 3 can convert into monomeric Pd(II) intermediate with an open coordination site, which had a higher activity. The end groups of the afforded polyfluorene were analyzed by matrix-assisted laser desorption ionization time-of-flight (MALDI-TOF) mass spectrometry, in which the Ar/H end groups are indicative of the catalyst-transfer polymerization. © 2015 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2015 , 53 , 1457–1463

研究领域: 高分子化学 · 有机合成 · 金属有机化学 · 功能材料 · 聚合反应机理
✓ 已验证 DOI 高影响因子
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RSC Advances · 2017 ·Vol. 7 ·期 59 ·36867-36875 · IF 3.108

Rational selection of halide ions for synthesizing highly active Au@Pd nanobipyramids

Fangyan Liu,Jia Ni,Hui Hao,Wei Wang,Wei Chen,Lijie Zhang,Chao Zou,Yun Yang,Shaoming Huang

Pd-based nanostructures with stepped facets possess potential applications in many fields, particularly in catalysis. Generally, crystal growth often only allows the formation of nanostructures with energetically non-stepped facets, so it is desirable to develop methods that can be used to prepare Pd-based nanostructures bounded by stepped facets. Herein, penta-fold twinned (PFT) Au@Pd nanobipyramids (NBs) with stepped {100} facets were synthesized through growing Pd on Au decahedral nanoparticles (NPs) in polyol. During the growth of Au@Pd NBs, Br− was a critical factor, because it has appropriate affinity for the Pd atom and adjusted the growth rate ratio along 〈110〉 and 〈100〉, resulting in the formation of Au@Pd NBs with stepped {100} facets. The product shape and size could be tailored by controlling the reaction conditions. Transmission electron microscopy (TEM), high resolution transmission electron microscopy (HRTEM), energy dispersive spectroscopy (EDS), high angle annular dark field (HAADF) imaging and scanning transmission electron microscopy EDS (STEM-EDS) were used to investigate the structure and growth of the Au@Pd NBs. A growth mechanism involving two stages was elucidated. In the first stage, the growth of Pd clearly occurred along both 〈110〉 and 〈100〉. In the second stage, the growth along 〈110〉 was faster than that along 〈100〉. Furthermore, we also demonstrated that the as-prepared Au@Pd NBs had high catalytic activity, compared with Pd nanocubes and Pd–Au–Pd segmental nanorods.

研究领域: 纳米材料化学 · 催化科学 · 无机合成 · 表面科学 · 电化学
✓ 已验证 DOI 高影响因子
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MICROCHIMICA ACTA · 2016 ·Vol. 183 ·期 8 ·2403-2409 · IF 4.831

Cyclovoltammetric acetylcholinesterase activity assay after inhibition and subsequent reactivation by using a glassy carbon electrode modified with palladium nanorods composited with functionalized C60 fullerene

Ye Cui,Zhong Xia,Wang Min-Qiang,Chai Yaqin,Yuan Ruo

A glassy carbon electrode (GCE) was modified with a nanocomposite consisting of tetraoctylammonium bromide (TOAB), C 60 fullerene, and palladium nanorods (PdNRs). The PdNRs were hydrothermally prepared and had a typical width of 20 ± 2 nm. The nanocomposite forms stable films on the GCE and exhibits a reversible redox pair for the C 60 /C 60 − system while rendering the surface to be positively charged. The modified GCE was applied to fabricate an electrochemical biosensor for detecting acetylcholinesterase (AChE) by measurement of the amount of thiocholine formed from acetylthiocholine, best at a working voltage of −0.19 V (vs. SCE). The detection scheme is based on (a) measurement of the activity of ethyl paraoxon-inhibited AChE, and (b) measurement of AChE activity after reactivation with pralidoxime (2-PAM). Compared to the conventional methods using acetylthiocholine as a substrate, the dual method presented here provides data on the AChE activity after inhibition and subsequent reactivation, thereby yielding credible data on reactivated enzyme activity. The linear analytical range for AChE activity extends from 2.5 U L −1 to 250 kU·L −1 , and the detection limit is 0.83 U L −1 . Cyclovoltammetric acetylcholinesterase (AChE) activity assay is constructed based on the palladium nanorods composited with functionalized C 60 fullerene (PdNR/C 60  + TOAB), which aims to measure the signal change between ethyl paraoxon-inhibited and subsequent pralidoxime (2-PAM)-reactivated AChE activity.

研究领域: 生物传感 · 酶学分析 · 纳米材料修饰电极 · 电化学检测 · 毒理学
✓ 已验证 DOI 高影响因子
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Nature Water · 2023 ·Vol. 1 ·期 1 ·95-103 · IF 0

Electrochemical hydrogenation of oxidized contaminants for water purification without supporting electrolyte

Xu Yinghua,Mao Zhechuan,Qu Ruifeng,Wang Jisheng,Yu Jianming,Luo Xingyu,Shi Meiqin,Mao Xinbiao,Ding Jie,Liu Bin

Electrocatalytic hydrogenation enables the efficient treatment of oxidized contaminants in water under mild conditions, but its application has been greatly hindered by the need for a supporting electrolyte and the large amounts of unsafe intermediate products. Here we report the development of a rhodium nanoparticle-modified palladium membrane electrochemical reactor (Rh NPs-PdMER) for the hydrogenation of oxidized contaminants in drinking water and industrial effluents. The Rh NPs-PdMER not only enabled the hydrogenation of 12 different oxidized contaminants to safe products with ≥99% conversion and ≥95% yield in water without a supporting electrolyte, but also required a very low operating voltage of only 1.4 V. The performance of the Rh NPs-PdMER can be attributed to the specific reactor configuration and the unique adsorbability of the hydrogenated intermediates of the oxidized contaminants to the Rh nanoparticles.

研究领域: 环境科学 · 水处理技术 · 电化学 · 纳米材料
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