Molecular Catalysis
·
2023
·
IF 4.6
Mengling Dong,Tao Li,Jiacheng Xu,Tiantian Zhang,Yan Sun,Ning Li,Zuliang Wu,Jing Li,Erhao Gao,Jiali Zhu,Shuiliang Yao,Yong Huang
Methane (CH 4 ) is the second largest greenhouse gas; its emission should be controlled. A plasma reactor coupled with a catalyst was used to control CH 4 emission via oxidation. Compared with the traditional catalytic process, the activity of Pd/ZrO 2 /Al 2 O 3 catalyst is significantly improved, the light-off temperature ( T 50 ) is at a level of 290 °C. X-ray photoelectron spectroscopy characterization results proved that synergetic effect of plasma and catalysis on CH 4 oxidation was due to the increase in the amount of lattice oxygen on zirconia after plasma oxidation and the enhancement of the oxidation of Pd 0 to PdO on 1.0Pd/10ZrO 2 /γ-Al 2 O 3 catalyst. An operando plasma diffuse reflectance infrared Fourier transform spectroscopy mass spectrometer was used to demonstrate that CH 4 oxidation on Pd/ZrO 2 /Al 2 O 3 catalyst. It was found that 1.0Pd/10ZrO 2 /γ-Al 2 O 3 with plasma can efficiently promote CH 4 oxidation and convert surface formate and carbonate to gaseous CO 2 and H 2 O. The plasma-generated O atoms can react with surface H 2 O to yield reactive OH radicals which can obviously improve CH 4 oxidation at a temperature higher than 130 °C, this finding provides important enlightenment for the development of catalysts for plasma catalytic oxidation of CH 4 . The mechanism of CH 4 plasma-catalysis oxidation was discussed.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Zuqin Duan,Xue Wang,Richu Wei,Qian Lei,Honglin Chen
A facile novel B, N co-doped carbon was fabricated by high-temperature pyrolysis of a mixture of ethylenediamine tetraacetic acid disodium salt and boric acid, on which Pd nanoparticles were loaded to synthesize highly efficient Pd/BNC catalyst for dehydrogenation of formic acid. The type and content of N are regulated by the doping of B elements in carbon materials. The high content of N and B doping provides more anchor sites for Pd and strengthens the interaction between the support and Pd nanoparticles, thus forming highly dispersed Pd nanoparticles and regulating the electronic property of Pd. Therefore, the obtained Pd/BNC catalyst displayed enhanced performance (TOF = 2760 h −1 ) and a lower activation barrier (31.84 kJ/mol). Furthermore, the catalyst also exhibited wonderful cycling stability for hydrogen evolution from formic acid.
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Molecular Catalysis
·
2023
·
IF 4.6
Weikun Chen,Xiao Fu,Xiaoying Liu,Linmin Ye,Youzhu Yuan
N -alkylated piperazines can be synthesized by the thermal catalytic alkylation of piperazine with alkyl halides or alcohols in the presence of supported metal catalysts. However, these processes either discharge large amounts of waste or require harsh conditions. Here, we report the results of N -alkylation of piperazine with lower alcohols (methanol, ethanol, and propanol) without external hydrogen addition at room temperature in the presence of a TiO 2 -supported Pd catalyst (Pd/TiO 2 -P) prepared by photodeposition method. Compared with the catalysts prepared by the conventional chemical reduction or hydrogen reduction, the Pd/TiO 2 -P catalyst showed the highest conversion of piperazine and the best selectivity to N -alkypiperazines. The mechanistic studies indicated that this phenomenon occurs via tandem photocatalytic reactions involving alcohol dehydrgenation to aldehyde, aldehyde condensation with piperazine to enamine, and enamine hydrogenation to N -alkylated piperazines. Considering the experimental results of methanol isotope kinetics, the α-C–H cleavage of methanol to form hydroxymethyl radical (·CH 2 OH) was proven to be the rate-determining step in the N -alkylation reaction of piperazine with low carbon alcohols. The characterization and control experiments revealed that the size of Pd nanoparticles and the valence of Pd species were vital to the reaction. The Pd/TiO 2 -P catalyst with an average of 2.5 ± 0.5 nm Pd particles and approximately 68% Pd 0 species on surfaces presented the highest activity for the photocatalytic tandem reactions of methanol dehydrogenation and enamine hydrogenation.
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Zhentao Li,Yanhui Fu,Qingsheng Zhu,Saijin Wei,Jie Gao,Yifu Zhu,Ting Xue,Ling Bai,Yangping Wen
Phosphorene (BP) is a rapidly rising star in two-dimensional (2D) layered nanomaterials beyond graphene, and its urgent issues of ambient instability still have to be resolved. Here, the bimetallic Pt-Pd nanoparticle on the BP surface was employed as multifunctional chemical and biochemical sensing platform for electrocatalytic detection of p -aminophenol (PAP), β-galactosidase (β-Gal), and Escherichia coli ( E. coli ). The BP-supported Pt-Pd nanoelectrocatalyst obtained by the electrodeposition of bimetallic Pt-Pd nanoparticle onto the BP surface was very stable in aqueous buffer containing oxygen, which displayed good voltammetric responses for PAP in a linear range of 0.02 -5 μmol·L -1 with a detection limit (LOD) of 1.41 × 10 −8 M and sensitivity 115.81 μA·μM -1 ·cm -2 . PAP could be obtained by the biochemical reaction of β-Gal in the presence of substrate PAP-β-galactopyranoside, which could realize for biochemical sensing of β-Gal in a linear range of 0.2 -0.8 mU·L -1 with a LOD of 9.35 nU·L -1 and sensitivity of 4.77 μA (mU·L -1 ) -1 ·cm -2 . The β-Gal is an indicator of total coliforms represented by E. coli that are induced by isopropyl-β-thiogalactopyranoside, which could applied for biochemical sensing of E. coli in a linear range of 6 × 106 –1.6 × 108 cfu·mL-1 with LOD of 6.65 × 10 5 cfu·mL -1 and sensitivity of 2.44 μA·(cfu·mL -1 ) -1 ·cm -2 . This work will provide experimental support for multifunctional chemical and biochemical sensing platform based on 2D layered nanomaterials decorated with bimetallic nanoelectrocatalysts.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Lian Duan,Chi Ma,Fengyan Lou,Jiabin Yin,Le Sang,Jisong Zhang
External mass transfer performance of micropacked bed reactors (μPBRs) with Pd/Al2O3/nickel foam catalysts is investigated by the hydrogenation of α-methylstyrene (AMS). The external mass transfer limitation region for AMS hydrogenation can be determined by means of the apparent activation energy and internal effectiveness factor. Parametric studies for external mass transfer are conducted by varying temperatures, operating pressures, liquid viscosities, gas and liquid superficial velocities, and pore diameters of foam packing. The external volumetric mass transfer coefficients [(ka)OV] of μPBRs with the Pd/Al2O3/nickel foam range from 0.06 to 0.71 s–1. An empirical correlation of (ka)OV is developed. Based on the gas–liquid–solid process analysis, the external mass transfer of μPBRs with the Pd/Al2O3/nickel foam is limited by liquid–solid mass transfer under the experimental conditions. Moreover, μPBRs with the Pd/Al2O3/nickel foam exhibit the best energy efficiency in comparison with that of other multiphase reactors.
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CARBON
·
2022
·
IF 11.307
Xiang Yu,Yue Zhan,Tingting Fan,Yuqi Zhang,Shunqin Liang,Limin Sun,Xiaoli Hu,Weiping Fang,Zhou Chen,Xiaodong Yi
The stabilization and transport of the reactants, intermediates and products are significant to rational design of an industrial catalyst. In this work, we encapsulated the surface of Pd/g-C 3 N 4 catalyst with acrylic acid (AA) using a photo-induced grafting method to mimic the 3-dimensional nature of enzymes. A combined characterization and ab initio calculation revealed that AA ligands on the surface controlled the adsorption and diffusion behaviors of the reactants, rather than alter the electronic or geometric properties of Pd active centers. The optimized catalyst (Pd/CNA-4) significantly enhances isoprene partial hydrogenation activity without a decline in semi-hydrogenation selectivity. This approach can be further optimized by changing the types of the encapsulating ligands and can meet other specific catalytic reactions to regulate their conversion and selectivity and is therefore expected to extend to other areas of heterogeneous catalysis .
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Chemical Science
·
2022
·Vol. 13
·期 46
·13956-13965
·
IF 9.969
Chen Wang,Wei Gao,Xinhao Wan,Bin Yao,Wenjing Mu,Jie Gao,Qiangang Fu,Dan Wen
Improving the utilization of noble metals is extremely urgent for fuel cell electrocatalysis, while three-dimensional hierarchical noble metal aerogels with abundant sites and channels are proposed to reinforce their electrocatalytic performances and decrease their amounts. Herein, novel Pd aerogels with tunable surface chemical states were prepared through a facile in situ electrochemical activation, starting with PdOx aerogels by the hydrolysis method. The hierarchical porous Pd aerogels showed unprecedented high activity towards the electrocatalytic oxidation of fuels including methanol (2.99 A mgPd−1), ethanol (8.81 A mgPd−1), and others in alkali, outperforming commercial catalysts (7.12- and 13.66-fold, corresponding to methanol and ethanol). Theoretical investigation unveiled the hybrid surface states with metallic and oxidized Pd species in Pd aerogels to regulate the adsorption of intermediates and facilitate the synergistic oxidation of adsorbed *CO, resulting in enhanced activity with the MOR as the model. Therefore, efficient Pd aerogels through the in situ electrochemical activation of PdOx aerogels were proposed and showed great potential for fuel cell anodic electrocatalysis.
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PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Zhuping Li,Yong Men,Shuang Liu,Jinguo Wang,Keye Qin,Dandan Tian,Tianle Shi,Li Zhang,Wei An
The crystalline phases of support have great influence on their surface and structure properties. Therefore, adjusting the crystalline structure of heterogeneous catalysts imposes a significant impact on the catalytic performance. Herein, a suite of Pd/In 2 O 3 /ZrO 2 catalysts with different crystalline phases of ZrO 2 were prepared and evaluated for CO 2 hydrogenation to CH 3 OH using the same amount of metal loading. The activity data showed the distinct superior reactivity of Pd/In 2 O 3 /ZrO 2 catalyst used mixed monoclinic and tetragonal phases ZrO 2 (Mix-ZrO 2 ) as support as compared to respective single phase of monoclinic ZrO 2 (m-ZrO 2 ) and tetragonal ZrO 2 (t-ZrO 2 ). The catalysts are extensively characterized through BET, XRD, HRTEM, UV–vis, H 2 -TPR, CO 2 /H 2 -TPD and XPS. Combining the characterization results and activity data, the superior activity of Pd/In 2 O 3 /Mix-ZrO 2 catalyst can be correlated with large particle size of Pd nanoparticles, the concentration of oxygen vacancies, and the abundant medium basic sites, which were essential for activation of H 2 and inert CO 2 and enhancement of catalytic performance. The best-performing Pd/In 2 O 3 /Mix-ZrO 2 catalyst exhibited a remarkable reactivity with space time yield (STY) of 0.54 g methanol ·h −1 ·g cat −1 at 573 K and 5 MPa, and stability without noticeable deactivation after 100 h of time on stream, demonstrating its potential as catalyst used in CH 3 OH synthesis from CO 2 hydrogenation.
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JOURNAL OF POROUS MATERIALS
·
2022
·Vol. 29
·期 5
·1479-1487
·
IF 2.523
Ye Tiantian,Liu Hanfang,Wang Fupeng,Xie Huijie,Ran Saisai,Xu Wei,Liu Jia,Li Bin,Lin Haifeng,Chai Yongming,Wang Lei
Here, we demonstrate a simple in situ synthesis of Pd@silicate-1 (S-1), using [Pd(NH 2 CH 2 CH 2 NH 2 ) 2 ]Cl 2 as a metal precursor and steam-assisted crystallization (SAC) method. The ultra-small Pd nanoparticles (NPs) (~ 1 nm) can be successfully in situ encapsulated into the silicate-1 matrix with well dispersion. The obtained Pd@S-1 catalyst possesses high crystallinity, a large specific surface area and pore volume. More importantly, Pd NPs encapsulated into silicate-1 matrix can avoid the aggregation and sintering during catalytic reaction. Meanwhile, micropores of silicate-1 can improve the selectivity of the products in the hydrogenation of biomass furfural. Consequently, Pd@S-1 catalyst shows excellent catalytic activity in the selective hydrogenation of biomass furfural with selectivity of 95.7% and activity of 83.7% in the condition of relatively low temperature (458 K). Therefore, this strategy provides a new idea for the synthesis of molecular sieve supported metal catalysts.
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INTERNATIONAL IMMUNOPHARMACOLOGY
·
2022
·
IF 5.714
Yu Chen,Jie Mei,Ping Zhang,Jiayu Liu,Lingyan Chen,Liwei Wu,Yan Zhang
IQ motif containing GTPase activating protein 1 (IQGAP1) is a scaffold protein to transduce multiple signals from the extracellular microenvironment. However, whether IQGAP1 mediates EGF-induced cancer progression has been not observed. In this research, we explored the immunological correlations of IQGAP1. IQGAP1 was up-regulated in most cancer and related to poor prognosis in ovarian cancer. In addition, IQGAP1 was correlated with immune-related genes and tumor-infiltrating lymphocytes. IQGAP1 was a novel EGF-response gene, which was up-regulated by EGF. As the downstream of EGFR, IQGAP1 mediated EGF-induced proliferation, migration and invasion of tumor cells and was essential for EGF-induced PD-L1 expression as well. Mechanically, IQGAP1 interacted with STATs and mediated their phosphorylation. Furthermore, Curcumin inhibited EGFR/IQGAP1 axis to down-regulate PD-L1 and suppress cancer progression. To sum up, IQGAP1 responds to EGF stimulation and mediates EGF-induced phosphorylation of STATs, which is a novel promising target for blocking the EGF-induced cancer progression.
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ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 32
·期 27
·2201872
·
IF 19.924
Yuan Zhou,Yang Yang,Xun Zhu,Tong Zhang,Ding-ding Ye,Rong Chen,Qiang Liao
Direct formic acid fuel cells (DFAFCs) possess the advantages of high power density and theoretical cell potential. Exploring robust catalysts for electrochemical formic acid electro-oxidation (FAO) is greatly essential for the wide spread uptake of DFAFCs. However, many electrodes with attractive catalysts suffer limited mass transport due to sluggish CO 2 bubble growth and departure steps on its surface. In this study, a superaerophobic electrode is developed by depositing fern-shaped palladium nanostructured arrays on the carbon paper (Pd-nanoarray@CP). Its unique superaerophobic feature successfully facilitates the CO 2 bubble releasing from the catalyst surface in a significantly small size. With the merits of specific nanoarray morphology, superior under water superaerophobicity, and rapid gas bubble release, the Pd-nanoarray@CP shows fast charge/mass transport rate, high electrocatalytic activity, and great stability for FAO. A direct formic acid fuel cell equipped with the Pd-nanoarray@CP anode is successfully fabricated on a microfluidic platform. A peak power density of 35.8 mW cm −2 and limiting current density of 173.3 mA cm −2 are obtained, respectively, which are 49.2% and 33.0% higher than that of conventional Pd-black anodes. The electrode with superaerophobic interface allows deeper insight into the mechanism of FAO efficiency and holds promise for possible applications of commercially viable DFAFCs.
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FUEL PROCESSING TECHNOLOGY
·
2022
·
IF 8.129
Xiang Li,Xiang Zeng,Ying Zhang
Bimetallic Pd-Ru/ hydroxyapatite (HAP) catalysts were developed together with Zirconium phosphate (ZrP) to prepare aviation fuel range hydrocarbons by one-pot HDO from lignocellulose-derived C15 oxygenate. The effects of the catalyst composition , reaction time, initial H 2 pressure and reaction temperature on the HDO were explored. 84.24% C8-C15 alkanes could be obtained by Pd 0.6 -Ru 1.8 /HAP at 150 °C, 4 MPa H 2 . The HDO pathway and the stability of the catalyst were also investigated. To explore the synergy of bimetals and the efficiency of the catalysts, a series of characterizations were conducted. The results verified that the bimetallic catalyst had a better adsorption capacity for the substrate, and the ruthenium external electron density raised due to the introduction of palladium , thereby enhancing the hydrodeoxygenation activity of the catalyst.
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