Catalysts
·
2019
·Vol. 9
·期 4
·387
·
IF 3.444
Bei Wang,Liu Tao,Yu Cheng,Fang Yang,Yuguang Jin,Chunmei Zhou,Hao Yu,Yanhui Yang
The direct alcohol fuel cell is a kind of power generation device that directly converts the chemical energy of small molecule alcohols into electric energy. In this paper, the electro-oxidation behaviors of some typical alcohols (methanol, ethanol, ethylene glycol, n-propanol, 2-propanol, and glycerol) over Pt, Pd, and Au electrodes were investigated in acidic, neutral, and alkaline media, respectively. By analyzing the activity information from a cyclic voltammetry (CV) method and some dynamic tests, several regularities were revealed in those electro-oxidation behaviors. Firstly, alkaline media is the best for the electro-oxidation of all these alcohols over Pt, Pd, and Au catalysts. Secondly, the hydrogen bond donation abilities (HBD) of different alcohols were found have a great relationship with the catalytic performance. In alkaline media, on Pt electrodes, the solute HBD is positively correlated with the ease of electrooxidation within the scope of this experiment. Contrarily, it is negatively correlated on Pd and Au electrodes. Additionally, for Pt catalysts in acidic and neutral media, the relationship becomes negative again as the HBD increases. Finally, the alcohol’s molecular structure properties were found to have a remarkably influence on the activity of different catalysts. Over the Pt electrode in alkaline media, the activation energy of methanol oxidation is 44.1 KJ/mol, and is obviously lower than the oxidation of other alcohols. Under similar conditions, the lowest activation energy was measured in the oxidation of n-propanol (14.4 KJ/mol) over the Pd electrode, and in the oxidation of glycerol (42.2 KJ/mol) over the Au electrode. Totally, among all these electrodes, Pt electrodes showed the best activities on the oxidation of C1 alcohol, Pd electrodes were more active on the oxidation of C2-3 monobasic alcohols, and Au electrodes were more active on the oxidation of polybasic alcohols.Keywords:DAFCs;electro-oxidation;gold;palladium;platinum
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SEPARATION SCIENCE AND TECHNOLOGY
·
2018
·
IF 1.2
Yan Yan,Qi Wang,Zeyang Xiang,Yanzhao Yang
A reasonable project was presented for the extraction and separation of Pt(IV), Pd(II), Ru(III), and Rh(III) from the mixed imidazolium-based ionic liquids (ILs) [C6mim]Cl, [C6mim][NTf2], and [C6mim][DDTC]. Pt(IV) was first separated from other three platinum group metals with a mixture of [C6mim]Cl and [C6mim][NTf2]. Then, separation of Pd(II) and Ru(III) from Rh(III) was realized by changing the concentration of [C6mim][DDTC]. Back-extraction of Pt(IV), Pd(II), and Ru(III) from loaded hydrophobic phase and the recovery of Rh(III) in aqueous phase were also investigated. Mechanisms between Pd(II)/Ru(III) and [C6mim][DDTC] were further explored using ultraviolet spectrophotometry (UV-Vis), infrared spectrophotometry (FTIR), the method of continuous variations, ab initio quantum chemical studies, and X-ray crystallographic analysis. The results afford more directions for extracting and separating metals by introducing devisable functionalized group into ILs.
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Journal of Materials Chemistry A
·
2016
·Vol. 4
·期 47
·18354-18365
·
IF 8.262
Lin Han,Pengfei Wang,Hui Liu,Qiangqiang Tan,Jun Yang
Tailoring the internal structure and chemical composition of nanomaterials is an effective way to enhance their performance for a given application. Herein, we report a general wet-chemistry approach to produce copper (Cu)-based binary hollow nanostructures with well defined architectures and investigate their catalytic properties in electrochemical reactions. This strategy relies on the galvanic replacement between Cu seeds and noble metal precursors including ruthenium (Ru), rhodium (Rh), palladium (Pd), osmium (Os), iridium (Ir), and platinum (Pt) in oleylamine at an appropriate temperature, which is essential to balance the reduction kinetics of the noble metal precursors by oleylamine during their galvanic replacement with Cu seed particles. Typically, the bimetallic CuPt hollow nanostructures with polyhedral morphologies exhibit enhanced catalytic properties for the oxygen reduction reaction (ORR), while their spherical counterparts obtained at a relatively low temperature show high activity for the methanol oxidation reaction (MOR). In particular, we will also demonstrate a unique application of the CuRu hollow nanostructures in supercapacitors after converting them into binary metal oxides at elevated temperatures in air.
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NEW JOURNAL OF CHEMISTRY
·
2017
·Vol. 41
·期 18
·10245-10250
·
IF 3.269
X. X. Wu,H. Zhou
Recently, porous carbon materials have attracted attention due to their versatile properties. In this study, a hierarchical porous N-doped carbon (NHPC) was successfully synthesized as a catalyst support using a facile method. A large amount of Pd nanoparticles were uniformly loaded on the NHPC with an average diameter of about 4.45 nm. The synthesized Pd/NHPC nanocatalyst exhibited excellent stability and reusability toward the reduction of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) at room temperature. The uniformity and high reusability of Pd/NHPC was mainly attributed to the abundant doped nitrogen as a coordinated site to largely stable Pd nanoparticles. Herein, the excellent properties of NHPC provided ideas for the fabrication of other NHPC supported noble nanoparticles, which can be applied in various catalytic reductive reactions.
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BIOSENSORS & BIOELECTRONICS
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2016
·
IF 7.476
Mingdang Li,Ping Wang,Faying Li,Qingyan Chu,Yueyun Li,Yunhui Dong
Herein, a novel and sensitive sandwich-type electrochemical immunosensor was fabricated for quantitative monitoring of prostate specific antigen (PSA). The sulfo group functionalized multi-walled carbon nanotubes (MWCNTs-SO 3 H) were used as substrate material to increase the specific surface area and enhance the conductivity of the glassy carbon electrode. Gold nanoparticles (Au NPs) were introduced to enhance the load capacity of the substrate material for primary antibodies (Ab 1 ) and accelerate the electron transfer on the electrode interface. The mesoporous core-shell Pd@Pt nanoparticle loaded by amino group functionalized graphene (M-Pd@Pt/NH 2 -GS) with high specific surface area, high indexed facets, and good biocompatibility was not only as the carriers of secondary antibodies (Ab 2 ) but also catalyzed the reduction of hydrogen peroxide (H 2 O 2 ), which effectually amplified the current signal in detection of PSA. The as-proposed immunosensor exhibited high sensitivity and stability on the detection of PSA. A linear relationship between current signals and the concentrations of PSA was obtained in the range from 10 fg/mL to 50 ng/mL and the detection limit of PSA was 3.3 fg/mL (signal-to-noise ratio of 3). Furthermore, the as-proposed immunosensor showed excellent performance in detection of human serum samples. The results suggest that the proposed immunosensor will be promising in the diagnostics application for accurately quantitative detection of PSA.
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Nano Research
·
2015
·Vol. 8
·期 10
·3237-3249
·
IF 7.01
Liang Ruowen,Jing Fenfen,Shen Lijuan,Qin Na,Wu Ling
Proper design and preparation of high-performance and stable dual functional photocatalytic materials remains a significant objective of research. In this work, highly dispersed noble-metal nanoparticles (Au, Pd, Pt) were immobilized on MIL-100(Fe) (denoted M@MIL-100(Fe)) using a facile room-temperature photodeposition technique. The resulting M@MIL-100(Fe) (M = Au, Pd, and Pt) nanocomposites exhibited enhanced photoactivities toward photocatalytic degradation of methyl orange (MO) and reduction of heavy-metal Cr(VI) ions under visible-light irradiation (λ ≥ 420 nm) compared with blank-MIL-100(Fe). Combining these results with photoelectrochemical analyses revealed that noble-metal deposition can effectively improve the charge-separation efficiency of MIL-100(Fe) under visible-light irradiation. This phenomenon in turn leads to the enhancement of visible-light-driven photoactivity of M@MIL-100(Fe) toward photocatalytic redox reactions. In particular, the Pt@MIL-100(Fe) with an average Pt particle size of 2 nm exhibited remarkably enhanced photoactivities compared with those of M@MIL-100(Fe) (M = Au and Pd), which can be attributed to the integrative effect of the enhanced light absorption intensity and more efficient separation of the photogenerated charge carrier. In addition, possible photocatalytic reaction mechanisms are also proposed.
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ANALYTICAL CHEMISTRY
·
2017
·
IF 6.32
Shouting Zhang,Dongxu Zhang,Xuehong Zhang,Denghui Shang,Zhonghua Xue,Duoliang Shan,Xiaoquan Lu
Herein, we developed a general strategy for rapid, highly selective, and ultratrace naked-eye colorimetric detection of Hg2+ in aqueous solutions. Two dimensional rGO/PEI/Pd nanohybrids, where rGO, PEI, and Pd were referred to as reduced graphene oxide, polyethylenimine, and Pd nanoparticles, respectively, were synthesized and used as mimetic peroxidase for selective and ultrasensitive detection of Hg2+ in water and human serum samples. In the presence of mercury ions, the peroxidase mimetic activity of rGO/PEI/Pd nanohybrids was found to be stimulated and enhanced significantly, which promoted the effective oxidation and color change of 3,3′,5,5′-tetramethylbenzidine (TMB) in solution to dark blue that was detected by the naked-eye and the absorption spectroscopic method. The proposed sensing strategy coupled with spectroscopic detection method showed an ultralow detection limit of 0.39 nM for Hg2+ in ddH2O and ∼1 nM in wastewater as well as serum samples, respectively. On the basis of the colorimetric assay, a minimum concentration of ∼10 nM for Hg2+ in wastewater and human serum can be detected with the naked-eye. The naked-eye-based colorimetric assay for sensitive and selective detection of mercury is expected to hold huge potentials in applications such as environmental monitoring, clinical diagnosis, and pharmaceutical analysis.
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IONICS
·
2024
·
IF 2.4
Duan Jinrong,Si Fang,Wang Jiafen,Lu Linlin,Liu Jia,Song Yanyan,Mo Jiahui,Yu Jincui,Gao Jinlong
Fuel cell is considered the best candidate power source because of its high energy conversion rate, large capacity, and zero emission. However, noble metal catalysts as a key core material have some problems, such as high cost and poor durability. Therefore, in this paper, the active self-supporting nanoporous Pd–Ag catalysts are successfully formed by cryogenic treatment and one-step dealloying treatment of Al-Pd–Ag ribbons. The surface of the catalyst ligaments shows a certain degree of preferred orientation for high-index facets (220) and (311). The results show that the activity and stability of the catalysts for methanol electrocatalytic oxidation are significantly improved under the synergistic effect of special configuration and promoter Ag. The electrocatalytic activity of the catalysts is about 9.7 and 15.2 times that of commercial Pt/C and commercial Pd/C catalysts, respectively. After 5000 s, the current density of the 1800 rpm-deep2 sample is 382.88 mA·mg −1 , which is about 14.1 times and 39.9 times that of commercial Pt/C catalyst and commercial Pd/C catalyst.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Fenglei Liu,Zhihao Li,Fang Xia,Baowei Hu
The efficient recovery of palladium from the spent nuclear fuel was of great significance to the sustainable development of nuclear energy. Herein, the uniform spherical COFs were constructed by a facile approach at room temperature, which were further surface functionalized by a thiol-ene “click” reaction to recover Pd(II). Microscopic and spectroscopic studies manifested that the formation mechanism and size of spherical COFs were greatly affected by the amount of catalyst and solvent type. The TAPB-BPTA-DTT and TAPB-BPTA-S-β-CD exhibited high Pd(II) recovery efficiency due to the introduction of sulfhydryl groups, and the maximum adsorption capacities were 489.3 and 234.3 mg/g, respectively. Meanwhile, the water environmental condition played an important role in the separation process, and the classical adsorption models demonstrated that monolayer chemisorption was the dominant removal mechanism. Mechanism analysis showed that the excellent adsorption performance was mainly attributed to the electrostatic interaction, physical absorption and chelation of N, O, and S groups with Pd(II). Thus, it is expected that this work could provide more insight into COFs materials, thereby promoting palladium removal advancements in the spent nuclear fuel.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Dongxuan He,Gang Wang,Binghan Li,Junrong Huang,Shuming Dou,Wei Gan,Hengzhi You,Qunhui Yuan
Tris(hydroxymethyl)aminomethane (Tris) and its derivatives serve as crucial biological buffers. Presently, Tris is predominantly synthesized by reducing tris(hydroxymethyl)nitromethane using conventional reducing agents such as hydrazine hydrate and metal powders. However, hydrazine hydrate poses a significant threat to aquatic life, while the use of reducing metal powders generates substantial solid waste, thereby exerting considerable environmental pressure in terms of green and sustainable chemistry. The utilization of non-homogeneous catalysts for hydrogenation reduction offers a viable solution to mitigate these issues. Yet, the exploration of non-homogeneous catalysts remains incomplete and lacks comprehensive research. In this study, a highly active Pd/C catalyst for the hydrogenation reduction of tris(hydroxymethyl)nitromethane was fabricated, through an ultrarapid high-temperature thermal shock (HTS) synthesis. The ultrafine Pd particles (∼5.5 nm) are uniformly distributed on the carbon substrate, rendering the catalyst high activity and stability. Additionally, we successfully combine this heterogeneous catalyst with continuous flow technology and achieve a continuous and stable production of Tris for more than 8 h, with a satisfying yield of ∼96%. This report may shed light on the efficient fabrication of more ultrafine catalysts for hydrogenation reductions with high noble-metal utilization.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Weizhen Xie,Chenting Yang,Quanwei Deng,Shigang Su,Lu Lin,Xing Tang
The selective hydrogenation of biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-bis(hydroxymethyl)tetrahydrofuran (BHMTHF) under mild conditions holds great significance for sustainable chemical production. However, this process remains hindered by challenges such as the instability of HMF in aqueous media and the insufficient efficiency of H 2 activation. Herein, a Pd catalyst supported on oxygen-vacancy–enriched MnO x -VC (Pd/MnO x -VC) is developed, featuring highly dispersed Pd/PdO heterostructures with abundant Pd–O–Mn interfacial active sites. Notably, Pd/MnO x -VC offered a high BHMTHF formation rates of 366.5 mol BHMTHF ·mol Pd −1 ·h −1 in water under mild conditions. Moreover, the catalyst was able to efficiently convert both purified and crude HMF at high concentrations (≥ 10 wt%), achieving BHMTHF yields exceeding 90 % in either batch or continuous-flow reactor under low temperatures (30–60 °C), underscoring its potential for industrial application. Mechanistic studies revealed that the relay activation of H 2 over Pd nanoparticles and adjacent Pd–O–Mn sites generates polarized H δ⁺ –H δ⁻ pairs, which primarily contributed to the outstanding activity of Pd/MnO x -VC. This work highlights the importance of interfacial site engineering in designing high-performance catalysts for HMF hydrogenation.
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Journal of Materials Chemistry B
·
2021
·Vol. 9
·期 43
·9031-9040
·
IF 6.331
Jilin Zheng,Peng Zhao,Shiying Zhou,Sha Chen,Yi Liang,Fengchun Tian,Jun Zhou,Danqun Huo,Changjun Hou
Integrating metal–organic frameworks (MOFs) of different components or structures together and exploiting them as electrochemical sensors for electrochemical sensing has aroused great interest. Furthermore, the incorporation of noble metals with MOFs is conducive to the improvement of catalytic performance. In this work, Pd@UiO-66-on-ZIF-L nanomaterials were successfully synthesised onto a self-supported flexible carbon cloth (Pd@UiO-66-on-ZIF-L/CC) through a novel strategy called MOF-on-MOF. Then, Au nanoparticles were electrodeposited onto Pd@UiO-66-on-ZIF-L/CC to obtain Au–Pd@UiO-66-on-ZIF-L/CC, which can serve as an excellent electrocatalyst for the reduction of hydrogen peroxide (H2O2). The obtained flower-like Pd@UiO-66-on-ZIF-L/CC hybrid MOF changes the structure of the monomeric MOF alone and adds more attachment sites. The synergy of the bimetals greatly improved the catalytic performance of the as-developed sensor. Electrochemical experiment results show that the proposed sensor based on Au–Pd@UiO-66-on-ZIF-L/CC has an extended linear range from 1 μM to 19.6 mM with a sensitivity of 390 μA mM−1 cm−2, and a low limit of detection (LOD) of 21.2 nM (S/N = 3). Moreover, it has good anti-interference, reproducibility, repeatability and excellent stability. Furthermore, the real-time in situ detection of H2O2 secreted from human adenocarcinomic alveolar basal epithelial cells (A549 cells) was achieved by culturing cells on Au–Pd@UiO-66-on-ZIF-L/CC, which indicates the potential of the sensor for applications in cancer pathology. Both the synthesis strategy and the sensor design provide new methods and ideas for the production of ultrasensitive H2O2 electrochemical sensors.
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