JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2020
·Vol. 95
·期 9
·2403-2410
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IF 2.75
Li Sun,Chuanliang Li,Hua Zhang,Binlin Dou,Wenxian Su,Lixin Zhang
BACKGROUND At present, much attention has been focused on the development of methane (CH 4 ) sensors due to a series of explosions and fires caused by CH 4 gas leakage. RESULTS Here, a CH 4 thermoelectric gas sensor (TGS) was fabricated by fixing 3D porous palladium/cobalt oxide (Pd/Co 3 O 4 ) catalyst on a commercial thermoelectric module. 3D porous Pd/Co 3 O 4 catalysts were prepared by a co-precipitation and gel-casting method. The pore structure in catalysts could be tailored only by adjusting the gel viscosity during the formation process. The protocol to tune the pore structure is facile and effective for the improvement of the activity of catalysts. By means of various techniques, the catalysts were characterized and then the possible catalytic mechanism was revealed. The CH 4 TGS based on the optimal Pd/Co 3 O 4 catalyst began to respond at 200 °C, following an obvious output voltage (Δ V ) of 5 mV. Enhancing the operating temperature to 240 °C, the value of Δ V reached to 31 mV and exhibited a linear relationship with CH 4 gas concentration. Meanwhile, the CH 4 TGS showed high sensitivity, repeatability and stability. CONCLUSION The easy and effective preparation method presented to prepare 3D porous Pd/Co 3 O 4 catalyst can provide an unique perspective on the development of 3D porous materials with excellent properties. It can be anticipated that the CH 4 TGS based on the 3D porous Pd/Co 3 O 4 catalyst will be a potential candidate for the detection of CH 4 gas in industrial settings. © 2020 Society of Chemical Industry
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Nanoscale
·
2020
·Vol. 12
·期 25
·13507-13512
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IF 6.895
Hongjing Wang,Songliang Liu,Hugang Zhang,Shuli Yin,You Xu,Xiaonian Li,Ziqiang Wang,Liang Wang
Electrochemical nitrogen reduction reaction (NRR) provides a facile and sustainable route to synthesize ammonia. The preparation of efficient and high-performance catalysts is one of the most important issues in large-scale applications of the electrochemical synthesis of ammonia. Herein, we have devised a simple method to fabricate three-dimensional palladium-silver-sulphur porous nanosponges (Pd–Ag–S PNSs) under room temperature. The porous network can provide more active sites and accessible channels for the reaction species. The incorporation of sulfur reduces the energy barrier of NRR and promotes the nitrogen hydrogenation to ammonia. Intrinsically, the Pd–Ag–S PNSs demonstrates a superior NRR performance with an NH3 yield of 9.73 μg h−1 mg−1cat. and a faradaic efficiency of 18.41% at −0.2 V, superior to those of the undoped Pd–Ag PNSs. The design of the three-dimensional metallic nanosponges with the doping of nonmetallic elements is a highly valuable strategy for NRR and other electrocatalytic reactions.
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高影响因子
JOURNAL OF CATALYSIS
·
2020
·
IF 7.888
Haiping Li,Tianxing Yang,Yiwei Jiang,Shuai Chen,Yufei He,Junting Feng,Dianqing Li
A feasible method for spontaneous in situ reductions on layered double hydroxides (LDHs) to prepare supported catalysts with Pd sub-nanoparticles is proposed. In this process, the reductive sites for the Pd 2+ are introduced into the LDHs laminates in a highly dispersed distribution, and a series of reductive supports (such as CoAl-LDHs, CoNiFe-LDHs, FeAl-LDHs) are prepared. The obtained reductive support is directly used to reduce Pd precursor without the addition of a reducing agent. HRTEM images show that metallic Pd is successfully reduced and evenly distributed on the support. Moreover, hexadecyl trimethyl ammonium chloride (CTAC) is introduced to improve the dispersion of Pd. HAADF-STEM results illustrate that metallic Pd particles are prepared in the form of a sub-nanometer size. XPS analysis show that Co and Pd species undergo a redox reaction and have an electronic interaction with CTAC. The factors affecting the nucleation and growth of Pd sub-nanoparticles in CTAC-modified support spontaneous in-situ redox are also discussed. The obtained Pd MI /CoAl-LDHs (prepared by modified support spontaneous in situ redox method (MI)) is applied to the selective oxidation of benzyl alcohol. It is found that the selectivity is 91% at a conversion of 92%, and turnover frequency (TOF) of Pd MI /CoAl-LDHs is 2.2 times higher than that of Pd D /MgAl-LDHs prepared by the common dipping method. Furthermore, Pd MI /CoAl-LDHs shows excellent stability in 5 times reusability and 150 h use, demonstrating the Oswald ripening of Pd particles can be effectively prevented.
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CATALYSIS LETTERS
·
2021
·Vol. 152
·期 5
·1407-1416
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IF 3.186
Hong Liang,Yang Jing,Li Yongzheng,Gao Xin,Song Wuling,Zhang Hongxi
Lignocellulosic biofuels are the most promising sustainable fuels for supplementing shrinking fossil resources. In this work, acid-modified vermiculite (AVM)-supported Pd–Ni bimetallic catalyst (Pd–Ni/AVM) was investigated for the hydrodeoxygenation of bio-oil and its model compounds to assess its reactivity. Pd–Ni/AVM was found to efficiently hydrodeoxygenate the investigated model compound (phenol). The phenol conversion reached 94% at 0.5% of Ni loading and temperatures beyond 513 K. Using these parameters, the phenolic hydroxyl group was removed, and the C = C bonds were saturated. This catalyst was also efficient in the hydrodeoxygenation of bio-oil. H 2 -TPR experiments elucidated the synergistic effects between the active component and the carrier, which were considered the main reason for the catalytic activity. Strong influences of the Ni loading and temperature on the hydrogenation of phenol were also observed when the Pd loading was fixed at 1 wt%. Graphic Abstract
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2021
·
IF 4.464
Shuang Dong,Zhou Yang,Baoliang Liu,Jintao Zhang,Peng Xu,Meng Xiang,Tong Lu
The research and develpoment of biomass waste derived carbon materials have attracted tremendous research interests in fabrication of high performance electrochemical sensors. In this work, noble metal NPs (i.e., Pd, Au and Ag) loading on Loofah sponge-derived well-ordered macroporous carbon (OMC)/ N -doped carbon thin layer (N-C) was designed by a general approach. This polydopamine (PDA)-based method has the advantages of simplicity, high efficiency and versatility. In virtue of the synergistic contribution from 3D macroporous carbon scaffold and highly active nobel metal NPs, these as-prepared Pd@OMC/N-C, Au@OMC/N-C and Ag@OMC/N-C electrode exhibit excellent electrochemical sensing performances for H 2 O 2 reduction, glucose oxidation and nitrite oxidation, respectively. Thus, 3D OMC/N-C loaded noble metal nanoparticles are promising materials for a wide spectrum of electrochemical sensor and biosensor applications.
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CHEMOSPHERE
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2021
·
IF 7.086
Yuan Chen,Yuancai Chen,Jianbo Jia,Bing Yan
The present study focuses on the successful preparation of microbial palladium nanoparticles (Pd-NPs). The even distribution of Pd in the periplasmic space of B. megaterium Y-4 cells is characterized using a transmission electronic microscopy (TEM) and scanning electron microscope (SEM). X-Ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD) revealed the domination of Pd (0) in Pd-NPs. The microbial Pd-NPs were selected to detoxify triclosan (TCS). Liquid chromatography-mass spectrometry (LC-MS) was used to analyze the intermediate products of dechlorination and oxidization. Free radicals quenching and 5,5-dimethyl-1-pyrroline N-oxide (DMPO) capturing experiments confirmed the crucial contribution of atomic H• and O 2 ·– to TCS degradation. Besides, TCS degradation by microbial Pd-NPs could alleviate the cytotoxicity of TCS polluted water. Meanwhile, great circulating utilization of microbial Pd-NPs was obtained in degrading TCS. Corresponding findings in the present study could provide new insight into the role of microbial Pd-NPs in detoxifying pollutants.
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CHEMICAL ENGINEERING SCIENCE
·
2019
·
IF 3.372
Tengda Wang,Jianxing Shan,Li Wang,Xiangwen Zhang,Guozhu Li
Aqueous-phase hydrogenation of 4-nitrophenol (4-NIP) by H 2 has been investigated in the presence of Pd nanoparticles (NPs) regulated by small biological molecules. Nucleosides and their derivatives were employed as capping agents of Pd NPs, and their effect on Pd activity was evaluated. All four kinds of nucleosides exhibited obvious promoting effect on the activity of Pd NPs in comparison to that without any capping agent. The general promoting effect sequence of nucleosides and their derivatives on the activity of Pd NPs was nucleoside ≥ nucleotide > deoxynucleoside > base > deoxynucleotide. The quantitative correlation between the activity promoting effect and the structure of nucleosides and their derivatives were also studied using the method based on poly-parameter linear free energy relationships. Moreover, the kinetic behaviors of 4-NIP hydrogenation over Pd NPs regulated by different nucleosides (adenosine, guanosine, cytidine, and β-thymidine) were studied systematically and different kinetic models were developed to fit the data. The obtained kinetic data fitted well to the Langmuir-Hinshelwood (L-H) model, where the surface reaction is the rate-controlling step. The apparent activation energy, adsorption enthalpy of 4-NIP, and dissociated adsorption enthalpy of hydrogen were calculated and compared for a better understanding of the mechanism. Pd NPs regulated by cytidine showed the lowest apparent activation energy of 43.66 kJ mol −1 .
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ELECTROANALYSIS
·
2019
·Vol. 31
·期 6
·1182-1188
·
IF 2.691
Faqiang Zhong,Zhiguang Liu,Yujie Han,Yujing Guo
In this work, the reduced graphene oxide functionalized with poly dimethyl diallyl ammonium chloride (PDDA) modified palladium nanoparticles (PDDA-rGO/Pd) had been facile synthesized and used as the sensing layer for sensitive determination of capsaicin. The prepared composite was characterized by transmission electron microscopy, UV-visible absorption spectroscopy. The image demonstrated that Pd nanoparticles were uniformly distributed on the graphene surface. The electrochemical properties of the prepared sensor were investigated by cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). The results showed that the nanocomposite exhibits attractive electrocatalytic activity towards the oxidation of capsaicin. This attributed to the synergistic action of the excellent properties of Pd nanoparticles and graphene nanosheets. Under optimized conditions, the electrochemical sensor possessed a dynamic linear range from 0.32 μM to 64 μM with a detection limit of 0.10 μM (S/N=3) for capsaicin detection. Moreover, the cost-effective and simple fabrication procedure, good reproducibility and stability as well as acceptable accuracy for capsaicin determination in actual samples are also the main advantages of this method, which might have broad application in other amide alkaloid detection.
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CHEMICAL ENGINEERING SCIENCE
·
2019
·
IF 3.372
Mingyue Liu,Renliang Huang,Chuanxi Li,Mingda Che,Rongxin Su,Shuzhou Li,Jing Yu,Wei Qi,Zhimin He
Nanoscale zero-valent iron has been widely applied in environmental remediation and toxic waste treatment, especially for the degradation of persistent organic pollutants (POPs). However, the dechlorination activity of Fe nanoparticles (Fe NPs) can be suppressed by the precipitation of iron oxides generated from the corrosion of Fe-Pd NPs under alkaline conditions, leading to a decreased dechlorination efficiency. Faced with this challenge, we report a highly effective dechlorination system that functions over a broad pH range and especially well under alkaline conditions in this work. Procyanidin (PROC), a natural polyphenol, was utilized as a stabilizer to manipulate the size distribution of Fe-Pd NPs and, more importantly, as a scavenger of Fe ions to prevent iron oxide precipitation. Experiments and theoretical calculations reveal that the generated Fe ions was mainly present in the form of bis- and tris-PROC-Fe complexes in the reaction solution. Compared with pristine Fe-Pd NPs, the PROC-modified Fe-Pd NPs had a dechlorination efficiency that was increased 20-fold (pH 9.0). Notably, a normalized rate constant was enhanced by more than 2 orders of magnitude compared to the previously reported dechlorination systems. The PROC-modified Fe-Pd NPs showed excellent dechlorination efficiency over a wide pH range (2.3–13.0).
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ACS Catalysis
·
2019
·
IF 12.221
Xingxing Li,Yu Pan,Hong Yi,Jingcheng Hu,Dali Yang,Fengzhi Lv,Wendian Li,Jinping Zhou,Xiaojun Wu,Aiwen Lei,Lina Zhang
Improving the selectivity and retaining the efficiency of catalysts are essential for industrial processes and remain a great challenge. Herein, we developed a facile route to synthesize Pd nanocubes (NCs) using Eosin Y as the photosensitizer under visible light. Subsequently, Pd NCs were uniformly loaded on N-doped carbon nanofibrous microspheres (NCMs) from carbonated chitin microspheres. This Pd NCs@NCM exhibited high reactivity and selectivity in alkyne semihydrogenation. For example, the hydrogenations of phenylacetylene to styrene and of 3-phenyl-2-propyn-1-ol to (Z)-cinnamyl alcohol were 12.9 and 18.3 times faster with Pd NCs@NCM than with Lindlar catalyst. According to the Mott–Schottky effect, loading of Pd NCs on N-doped carbon constructed a rectifying contact and decreased the electron density of Pd NCs. Density functional theory (DFT) calculations suggested that the high concentration of holes doped in Pd NCs weakened the interaction of alkenes on the Pd (100) facet and prevented further hydrogenation for a long time; this period of durable time is very helpful in chemical manufacturing. Thus, Pd NCs@NCM maintained both high reactivity and selectivity in comparison with surface-modified catalysts. This work provides an alternative strategy to design Mott–Schottky catalysts for selective hydrogenation reactions.
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ACS Nano
·
2019
·
IF 13.903
Jinchang Fan,Xiaoqiang Cui,Shansheng Yu,Lin Gu,Qinghua Zhang,Fanqi Meng,Zhangquan Peng,Lipo Ma,Jing-Yuan Ma,Kun Qi,Qiaoliang Bao,Weitao Zheng
Rational control of the components of noble metal alloys is paramount for achieving satisfactory electrocatalytic performances. Though transition metals are commonly used to modify noble metals, many potential elements remain to be explored. Here, we interstitially modulate hydrogen atoms into RhPd nanoparticles to boost the alkaline hydrogen evolution reaction (HER). The obtained stable RhPd-H nanoparticles exhibit pronounced alkaline HER activity with a small overpotential of 36.6 mV at 10 mA cm–2 and a low Tafel slope of 35.3 mV dec–1. The surface electronic state, bond distance, and coordination number of the Rh and Pd atoms are significantly influenced by the presence of interstitial hydrogen atoms. These modifications give RhPd-H nanoparticles a desirable hydrogen adsorption free energy, thus accelerating the hydrogen gas production. We further demonstrate that the interstitial hydrogen atom modulation strategy to improve the HER activity is universal for other Pd-based alloy nanostructures. This work presents a powerful strategy for designing efficient electrocatalysts for the HER and beyond.
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Nano Research
·
2018
·Vol. 11
·期 6
·3272-3281
·
IF 7.994
Cai Shuangfei,Liu Xueliang,Han Qiusen,Qi Cui,Yang Rong,Wang Chen
We report a facile protocol for the one-pot preparation of monodisperse Pd nanoparticles (NPs) supported on ultrathin NiCl 2 nanosheets (NSs). The effective protocol can be described as in situ reduction–oxidation–assembly to create Pd/NiCl 2 nanocomposites and is applicable for the development of stable yet highly active Pd-based heterogeneous catalysts for organic transformations. The Pd/NiCl 2 composite displayed synergistically enhanced catalytic activity, high stability, and good recyclability for the tested model oxidation reaction. The in situ nucleation and growth of NiCl 2 NS around Pd NPs guaranteed a clean metal–support interface and greatly facilitated the catalytic reaction. This work provides a novel synthesis method for supported Pd nanocomposites suitable for many important applications.
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