ACS Applied Energy Materials
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2024
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IF 5.4
Tao Chen,Manli Wang,Donghang Hu,Qianlin Ju,Kaige Zhao,Liang Fu,Zelin Chen,Xiaolong Yu,Changjiu Li
The mainstream electrocatalysts for direct ethanol fuel cells (DEFCs) are Pt- or Pd-based nanomaterials, which are severely hampered by CO intermediate poisoning and the relatively low selectivity of the C1 pathway in anodic ethanol oxidation reaction (EOR), thereby impeding the efficiency enhancement and practical application of DEFCs. Herein, we report a Pt-decorated amorphous PdS nanowire [denoted as a-Pd(S)NWs/Pt] catalyst with abundant crystalline/amorphous heterogeneous interfacial active sites for alkaline EOR. The a-Pd(S)NWs/Pt was demonstrated a superior EOR mass activity of 6.16 A·mgPd+Pt–1, which is 22.81 times over that of commercial Pt/C (0.27 A·mgPt–1) and 34.22 times over that of commercial Pd/C (0.18 A·mgPd–1). Additionally, the a-Pd(S)NWs/Pt exhibited considerable stability, significantly enhanced resistance to CO poisoning and enhanced selectivity for the EOR C1 pathway. Density functional theory calculations and experimental results further revealed that the optimized COads and OHads binding energies due to the decoration of Pt nanoclusters can be responsible for the enhanced CO resistance and C1 selectivity of a-Pd(S)NWs/Pt. Furthermore, benefiting from its optimized electronic configuration at the interfacial active sites and the appropriate intermediate adsorption capacity, the a-Pd(S)NWs/Pt electrocatalyst was successfully extended to the electrocatalytic methanol and ethylene glycol oxidation reaction systems.
研究领域:
材料科学
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电化学
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催化
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DOI
高影响因子
CATALYSIS TODAY
·
2024
·
IF 5.2
Min Qiao,Jiansu Ran,Tianyi Yang,Zhaohui Liu,Kexin Yao
Resorcinol 1,4-phthalaldehyde resin (RPR) was successfully synthesized using a solvent-free self-assembly method employing a template (F127) and a mixture of resorcinol and 14-phthalaldehyde. After the removal of the template (F127) by heating, the PRR exhibited an ordered mesoporous structure with a size of approximately 5.8 nm. After impregnating with Pd species, a RPR supported Pd catalyst (Pd/RPR) was finally obtained, which demonstrated outstanding catalytic performance and good stability in the hydrodeoxygenation of vanillin . With an optimal catalyst, 100% conversion of vanillin and 96.7% selectivity for 2-methoxy-4-methylphenol were achieved under the reaction conditions of 2 MPa H 2 in ethanol at 90 ℃ over 4 hours. The superior catalytic properties of Pd/RPR with high activity and stability are anticipated to be significant for future biofuel upgrades.
研究领域:
化学工程
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材料科学
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DOI
高影响因子
Journal of Materials Chemistry A
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2021
·Vol. 9
·期 25
·14507-14514
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IF 12.732
Wenyan Si,Ze Yang,Xiuli Hu,Qing Lv,Xiaodong Li,Fuhua Zhao,Jianjiang He,Changshui Huang
Zero valence palladium (Pd(0)) nanoparticles have been reported to be more favorable to the oxygen reduction reaction (ORR) than palladium oxide (PdO). However, PdO is normally concomitant in Pd(0) nanoparticles. Herein, we developed an inventive method to prepare pure Pd(0) nanoparticles supported with hydrogen-substituted graphyne (Pd/HsGY) and its nitrogen-doped sample (Pd/N–HsGY). Pd(0) nanoparticles were obtained by reducing the atomically dispersed bivalent Pd, which is easy to be anchored on HsGY. The unique sp-hybridized carbon atoms in HsGY exhibited obvious extrinsic charge compensation to maintain the supported Pd nanoparticles to zero valence state. The as-prepared samples, especially Pd/N–HsGY, displayed excellent activity for ORR, higher than that of commercial Pd/C and Pt/C. In an alkaline medium, the mass activity of Pd/N–HsGY at 0.8 V (vs. RHE) was 2.1 times higher than that of Pd/C, and 1.7 times higher than that of Pt/C. While in an acidic medium, the mass activity of Pd/N–HsGY was 17.7 and 1.6 times Pd/C and Pt/C, respectively. Pd/N–HsGY based Zn–air battery exhibited higher power density than Pt/C-based battery and superior stability for more than 300 hours. Density functional theory calculations confirmed that Pd(0) nanoparticles, Pd/HsGY and Pd/N–HsGY were favorable to ORR. This method brings new perspectives for designing zero valence metal nanoparticles for electrocatalytic applications.
研究领域:
材料科学
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电化学
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催化科学
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DOI
高影响因子
Molecular Catalysis
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2019
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IF 2.938
Xinli Tong,Zhenya Zhang,Yiqi Gao,Yue Zhang,Linhao Yu,Yongdan Li
A novel carbon-chain increasing valorization of furfural (FUR), a cheap bio-based platform compound, has been successfully performed via the catalytic oxidative condensation process with mono-dispersed palladium oxide catalyst. For the reaction of furfural, n-propanol and O 2 , the PdO@TiO 2 exhibited a prominent catalytic activity in which a 77.8% conversion of FUR with 89.2% selectivity of 3-(furan-2-yl)-2-methylacrylaldehyde was obtained. Based on the XRD, SEM, TEM, HRTEM, XPS, and UV–vis results of catalysts, it was concluded that high activity is associated with particle size, uniform distribution of palladium oxide and surface area of the support. Moreover, the recycling experiments confirmed that mono-dispersed palladium oxide catalyst was stable, in which it still kept a good catalytic performance after being recycled for five times. This provided a new route for the selective transformation of the hemicellulose-derived platform compounds.
研究领域:
催化化学
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可再生化学
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材料科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2017
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IF 6.216
Shuang Zheng,Pengyong Yang,Fumin Zhang,De-Li Chen,Weidong Zhu
Pd nanoparticles encaged within an amine-functionalized metal-organic framework (MOF), Pd@NH 2 -UiO-66, was successfully prepared via one pot direct construction of the MOF framework, cooperative in situ metal precursor incorporation followed by on-site moderate reduction process. Because of its abundant of nanocages accessible through small pore windows, as well as excellent coordination capability of metal ions sites from the amine groups within the NH 2 -UiO-66 matrix, the Pd nanoparticles were homogeneously confined within its cavities. Intriguingly, the prepared Pd@NH 2 -UiO-66 exhibits a high catalytic activity and exclusive selectivity in the liquid-phase hydrogenation of 2,3,5-trimethylbenzoquinone (TMBQ) to 2,3,5-trimethylhydroquinone (TMHQ), a key vitamin-E intermediate in a short period under relatively mild reaction conditions. Additionally, this catalyst was recycled up to 8 times without significant loss in both activity and selectivity. Furthermore, reaction mechanism was investigated using dispersion corrected density functional theory calculations, suggesting that the superior performance of Pd@NH 2 -UiO-66 could be ascribed to the cooperation between the Pd nanoparticle and the amine-functionalized UiO-66. This MOF-based composite shows great potential as heterogeneous catalyst for the catalytic hydrogenation reactions due to its high stability, excellent catalytic properties, and simple preparation.
研究领域:
化学
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材料科学
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催化反应机制
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DOI
高影响因子
JOURNAL OF POWER SOURCES
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2015
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IF 6.217
Xiangheng Niu,Hongli Zhao,Minbo Lan
Methanol, a high-energy substance, is widely used for green fuel cells. However, the sluggish electrochemical methanol oxidation reaction (MOR) on state-of-the-art catalysts still requires for exploring high-performance and low-cost materials to further promote the reaction kinetics at low overpotentials. Here we carried out the first electrocatalytic comparison study of two Ni foam-supported Pd nanomaterials (Pd-2-Ni and Pd-4-Ni, respectively), obtained through the spontaneous galvanic replacement of Ni with different palladic precursors ([PdCl 4 ] 2- and [PdCl 6 ] 2− , respectively), toward MOR. With replacement, Pd deposits with discrepant arrangements and coverages were grown on the porous Ni support. Compared to commercial Pd/C, both Pd-2-Ni and Pd-4-Ni exhibited better mass activity and catalytic durability for MOR in alkaline media . More interestingly, different palladic precursors made a significant effect on the catalytic performance of the Ni foam-supported Pd deposits. In Pd-4-Ni, the 2:1 stoichiometric replacement of Ni with [PdCl 6 ] 2− enabled the incompact arrangement of Pd structures, with more exposure of Ni atoms adjoined to Pd atoms on the catalytic interface compared to Pd-2-Ni. As a result, with the favorable Ni-neighbor-Pd regime and the higher utilization efficiency of Pd atoms, the synthesized Pd-4-Ni catalyst provided a mass activity of approximately 1.5 times higher than Pd-2-Ni toward MOR.
研究领域:
材料科学
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电化学
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催化
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能源材料
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DOI
高影响因子
Applied Sciences-Basel
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2019
·Vol. 9
·期 9
·1792
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IF 2.217
Anqiu Liu,Xiaochen Wang,Daming Gao,Le Wang,Junjie Cheng,An Wang,Zehui Zhang
Chemoselective hydrogenation of aldehydes with heterogeneous catalysts under mild conditions is of great importance but remains a major challenge. Herein, an efficient strategy was developed for low temperature chemoselective hydrogenation of aldehydes with broad substrate scope over a magnetic material supported palladium catalyst (γ-Fe2O3@HAP-Pd). Aldehydes bearing various reducible functional groups readily underwent hydrogenation to give the corresponding primary alcohols with moderate to excellent yield at room temperature in aqueous solutions. The Hammett equation revealed that the hydrogenation of aromatic aldehydes proceeded via an anionic intermediate. Additionally, when the temperature increased to 70 °C, toluene was obtained by the deoxygenation of benzaldehyde in excellent yield. Furthermore, the γ-Fe2O3@HAP-Pd could be recycled up to six times without loss of activity and metal leaching.Keywords:selective hydrogenation;aldehydes;Pd catalysts;mild conditions
研究领域:
催化化学
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材料科学
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DOI
高影响因子
Nanomaterials
·
2018
·Vol. 8
·期 3
·141
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IF 3.504
Guangyin Fan,Xiaojing Li,Caili Xu,Weidong Jiang,Yun Zhang,Daojiang Gao,Jian Bi,Yi Wang
Developing highly efficient and recyclable catalysts for the transformation of toxic organic contaminates still remains a challenge. Herein, Titanium Carbide (Ti3C2) MXene modified by alkali treatment process was selected as a support (designated as alk-Ti3C2X2, where X represents the surface terminations) for the synthesis of Pd/alk-Ti3C2X2. Results show that the alkali treatment leads to the increase of surface area and surface oxygen-containing groups of Ti3C2X2, thereby facilitating the dispersion and stabilization of Pd species on the surface of alk-Ti3C2X2. The Pd/alk-Ti3C2X2catalyst shows excellent catalytic activity for the hydrodechlorination of 4-chlorophenol and the hydrogenation of 4-nitrophenol in aqueous solution at 25 °C and hydrogen balloon pressure. High initial reaction rates of 216.6 and 126.3 min−1·gpd−1are observed for the hydrodechlorination of 4-chlorophenol and hydrogenation of 4-nitrophenol, respectively. Most importantly, Pd/alk-Ti3C2X2exhibits excellent stability and recyclability in both reactions without any promoters. The superior property of Pd/alk-Ti3C2X2makes it as a potential material for practical applications.Keywords:palladium;titanium carbide;catalytic transformation;4-chlorophenol;4-nitrophenol
研究领域:
材料科学
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环境科学
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催化化学
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DOI
PubMed
高影响因子
Nuclear Science and Techniques
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2020
·Vol. 31
·期 4
·1-13
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IF 1.556
Zhang Shi-Chang,Ning Shun-Yan,Zhou Jie,Wang Si-Yi,Zhang Wei,Wang Xin-Peng,Wei Yue-Zhou
A porous silica-polymer-based adsorbent, iso Bu-BTP/SiO 2 -P, was prepared by a vacuum impregnation method and used for the recovery of ruthenium, rhodium, and palladium from nitric acid solution. The experimental results revealed that iso Bu-BTP/SiO 2 -P exhibited unique adsorption properties such as high saturation adsorption capacity (Ru: 0.35 mmol g −1 , Rh: 0.32 mmol g −1 , Pd: 1.05 mmol g −1 ) and excellent selectivity over other metal ions, such as lanthanides (SF PGM/ M > 40) in 1 M HNO 3 solution. The adsorption process conformed to the pseudo-second-order model and Langmuir model. From the UV, FTIR, and XPS analyses, it can be concluded that the strong affinity between functional groups (C–N=C) and metal ions as well as NO 3 − played a role in coordination during the adsorption process. Furthermore, the desorption behavior was studied, and it was found that the adsorbed Pd, Rh, and Ru could be eluted with a 0.01 M nitric acid–0.1 M thiocarbamide solution, 5 M hydrochloric acid, and sodium hypochlorite (CP) solution, respectively. Finally, based on those findings, a simple process for the separation and recovery of Pd, Rh, and Ru from high-level liquid waste using iso Bu-BTP/SiO 2 -P was designed and proposed.
研究领域:
化学工程
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材料科学
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DOI
高影响因子
JOURNAL OF POLYMERS AND THE ENVIRONMENT
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2024
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IF 4.7
Liu Yaqing,Cui Yixin,Meng Huibiao,Long Ke,Shao Linjun,Xing Guiying
Palladium plays an important role in modern industry, agriculture and medicine. The direct discharge of palladium results in serious environmental pollution and loses of precious palladium metal. Herein, kaolin/chitosan hybrid nanofibers were successfully prepared to recover Pd 2+ cations from aqueous solution. Chitosan and kaolin mixture was first electrospun into nanofibers with citric acid as the in situ crosslinking agent and poly(ethylene oxide) as the co-spinning polymer. Then, the chitosan molecules in these hybrid nanofibers were in situ crosslinked by critic acid at elevated temperatures to endow these nanofibers with excellent solvent resistance. Their structure characterization was conducted by Fourier-transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM) and positron annihilation lifetime spectroscopy (PLAS). The adsorption performances of these fibrous adsorbents were carefully investigated and optimized (e.g. kaolin content, temperature, pH of solution and initial Pd 2+ concentration). The adsorption results demonstrated that incorporation of kaolin powders into the nanofibers could enhance the adsorption capacity from 31 mg/g to 64 mg/g. Thermodynamic parameters studies revealed the endothermic and spontaneous natures of the adsorption process of Pd 2+ cations on these hybrid nanofibers. The Pd 2+ adsorption behavior of this fibrous adsorbent fitted well with the second-order kinetic model, suggesting the chemical adsorption behavior of Pd 2+ cations on this fibrous adsorbent. Moreover, this fibrous adsorbent can be easily regenerated and reused at least three times without significant loss of initial adsorption capacities. These results clearly indicate that this fibrous chitosan/kaolin hybrid absorbent holds great potential in the recovery of precious palladium cations from aqueous solution.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
ACS ES&T Engineering
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2022
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IF 0
Jiazhen Cao,Yao Chen,Hengjun Shang,Xiang Chen,Qianyu Qiao,Hexing Li,Zhenfeng Bian
Gold and palladium are the most widely used precious metal materials in the field of electronic devices and industrial catalysis. How to realize the green recycling of gold and palladium is important and challenging. In this work, we found that gold and palladium in wastes, such as electronic devices and industrial catalysts, can be completely dissolved and recycled by photocatalysis. Gold and palladium are oxidized to the ionic state in water, which does not involve strong acids, strong alkalis, toxic cyanides, or an organic medium. More interestingly, the dissolution of gold and palladium in different halogen aqueous solutions has special selectivity, which depends on the coordination stability constants between gold and palladium with halide ions. Therefore, gold and palladium can be selectively dissolved in iodine ion solution and bromine ion solution, respectively, then gold and palladium can be obtained by a one-step reduction. This work opens up a new direction for optimizing the photocatalytic dissolution technology and promoting the green recycling of precious metals.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
Arabian Journal of Chemistry
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2020
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IF 4.762
Zhen Huang,Chen Wang,Jiling Zhao,Shixing Wang,Yang Zhou,Libo Zhang
A new adsorbent was successfully fabricated by chemically linking pyromellitic acid onto a zirconium-based metal-organic framework composite for selective adsorption of Pd(II) from an aqueous solution. The adsorbent was characterized by Fourier transform infrared spectroscopy, Brunauer–Emmett–Teller equation and scanning electron microscope. The adsorption capacity, selectivity and repeatability of the adsorbent were tested by batch experiments. The optimum pH was 2.0, and the maximum adsorption capacity at room temperature was 226.1 mg/g. In the kinetic experiments, the adsorption process achieved equilibrium within 5 h and generally conformed to the quasi-second kinetics and Freundlich isotherm model. The N-H and O H groups on the adsorbent interacted with Pd(II) by electrostatic and coordination action. The adsorbent maintained excellent adsorption capacity after at least 5 cycles. At the same time, the selectivity of the adsorbent in aqueous solution is excellent from interfering ions. Therefore, the new adsorbent will have an obvious application prospect on the recovery of palladium.
研究领域:
化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）