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Journal of Environmental Sciences · 2022 · IF 6.796

Nano-sized alumina supported palladium catalysts for methane combustion with excellent thermal stability

Wei Shi,Guangyan Xu,Xuewang Han,Yingjie Wang,Zhi Liu,Sen Xue,Nannan Sun,Xiaoyan Shi,Yunbo Yu,Hong He

Pd/Al 2 O 3 catalysts supported on Al 2 O 3 of different particle sizes were synthesized and applied in methane combustion. These catalysts were systematically characterized by Brunauer-Emmett-Teller (BET), X-ray diffraction (XRD), high resolution-transmission electron microscopy (HR-TEM), high-angle annular dark field-scanning transmission electron microscopy (HAADF-STEM), H 2 -temperature-programmed reduction (H 2 -TPR), O 2 -temperature-programmed oxidation (O 2 -TPO), X-ray photoelectron spectroscopy (XPS), and X-ray absorption fine structure (XAFS). The characterization results indicated that nano-sized Al 2 O 3 enabled the uniform dispersion of palladium nanoparticles , thus contributing to the excellent catalytic performance of these nano-sized Pd/Al 2 O 3 catalysts. Among them, Pd/Al 2 O 3 -nano-10 (Pd/Al 2 O 3 supported by alumina with an average particle size of 10 nm) showed superior catalytic activity and stability for methane oxidation under harsh practical conditions. It maintained excellent catalytic performance for methane oxidation for 50 hr and remained stable even after harsh hydrothermal aging in 10 vol.% steam at 800°C for 16 hr. Characterization results revealed that the strong metal-support interactions and physical barriers provided by Al 2 O 3 -nano-10 suppressed the coalescence ripening of palladium species, and thus contributed to the superior sintering resistance of the Pd/Al 2 O 3 -nano-10 catalyst.

研究领域: 催化化学 · 材料科学
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APPLIED SURFACE SCIENCE · 2021 · IF 6.707

Confinement of ultrasmall Pd nanoparticles by layered covalent triazine frameworks for semihydrogenation of acetylene

Jiqiu Zhang,Guanyin Zhang,Liang He,Yuzhen Shi,Rongrong Miao,Yuanzhi Zhu,Qingqing Guan

Acetylene hydrogenation is an important reaction in the petrochemical industry, the key is to develop efficient and selective catalyst. In this work, a highly crystalline layered covalent triazine frameworks (CTFs) with excellent thermal stability was used as carbon support to immobilize ultrasmall Pd nanoparticle for semihydrogenation of acetylene. Downsizing the particle sizes were realized by dual-solution assisted precursor mixture and using H 2 instead of NaBH 4 as reducing agent. The pore confinement effect of CTFs and the electronic intercalation from N atoms play key roles in improving the catalytic activity and stabilizing the Pd nanoparticles. The Pd/CTFs-H 2 catalyst exhibits 100% acetylene conversion and 99.9% ethylene selectivity at 250 °C and space velocity of 110,000 h −1 . The life test (>150 h), cycle test and chemical stability test demonstrated the long-term stability of the Pd/CTFs-H 2 . The process mechanism of selective hydrogenation of acetylene in this catalyst is investigated by the in-situ infrared spectra .

研究领域: 材料科学 · 催化化学
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Physica Status Solidi-Rapid Research Letters · 2022 ·Vol. 16 ·期 6 ·2200017 · IF 3.277

High-Performance Humidity Sensor Based on CsPdBr3 Nanocrystals for Noncontact Sensing of Hydromechanical Characteristics of Unsaturated Soil

Sheng Huang,Husheng Shan,Wufan Xuan,Wenjie Xu,Dunan Hu,Lei Zhu,Cheng Huang,Wanghua Sui,Chunjin Xiao,Yulong Zhao,Yinghuai Qiang,Xiuquan Gu,Jian Song,Chang Zhou

The humidity sensors based on metal halide perovskite have achieved outstanding improvement. However, there are few reports of perovskite nanocrystals for humidity sensors. Herein, CsPdBr 3 nanocrystals with high surface-to-volume ratio are synthesized by the in situ spin-coating method. Subsequently, the humidity sensor based on CsPdBr 3 nanocrystals is prepared and the response mechanism is demonstrated to originate from the formation of the Pd––O bond on the surface by performing density functional theory calculation. The humidity sensor shows a fast response/recovery time of 0.68/2.43 s in a relative humidity range from 88.9%RH to 4.7%RH; the fast response/recovery properties are used to monitor human respiratory and noncontact switch. Moreover, the hydromechanical characteristics of unsaturated soil are obtained by noncontact testing with the humidity sensor for the first time in geological engineering, and the strong correlation between relative humidity and hydromechanical characteristics is revealed by mathematical derivation, which lays the theoretical foundation for the noncontact real-time sensing of hydromechanical characteristics of unsaturated soil. These findings not only open the door to the development of perovskite nanocrystals materials for humidity measurement, but also offer a new method for nondestructive and real-time test of the mechanical properties of soil in geological engineering.

研究领域: 材料科学 · 地质工程 · 传感器技术
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RSC Advances · 2016 ·Vol. 6 ·期 43 ·37118-37123 · IF 3.289

Palladium nanoparticles embedded in metal–organic framework derived porous carbon: synthesis and application for efficient Suzuki–Miyaura coupling reactions

Wenhuan Dong,Li Zhang,Chenhuan Wang,Cheng Feng,Ningzhao Shang,Shutao Gao,Chun Wang

A nanoporous carbon (NPC) material was prepared by one-step direct carbonization of a metal–organic framework, MOF-5, without additional carbon precursors. Pd nanoparticles were immobilized on the MOF-5-derived NPC by an impregnation method coupled with subsequent reduction with NaBH4. The prepared catalyst was in-depth characterized by X-ray photoelectron spectroscopy, transmission electron microscopy, scanning electron microscopy, and N2 adsorption. The catalyst was used to catalyze the Suzuki–Miyaura coupling reactions and exhibited high catalytic efficiency with yields ranging from 90% to 99% under mild conditions. The results demonstrated the great application potential of MOF precursor-based metal nanoparticle composites in catalysis.

研究领域: 材料化学 · 纳米催化 · 多孔材料 · 有机合成方法学 · 能源与环境材料
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CERAMICS INTERNATIONAL · 2019 ·Vol. 45 ·期 10 ·13150-13157 · IF 3.45

Enhanced CH4 sensing properties of Pd modified ZnO nanosheets

Yan Wang,Xiaoning Meng,Mengxia Yao,Guang Sun,Zhanying Zhang

In this paper, pristine ZnO and Pd modified ZnO nanosheets have been successfully prepared via a facile hydrothermal route and the subsequent calcination process. The composition, morphology and nanostructure of the as-obtained materials were characterized by X-ray diffraction (XRD), field-emission scanning electron microscopy (FESEM) and transmission electron microscopy (TEM). The methane (CH 4 ) sensing properties of Pd/ZnO were compared with those of pure ZnO , and the materials showed the noticeable sensing capability when the loading amount of Pd was 1 at%. Moreover, the optimal working temperature of ZnO was reduced from 240 °C to 200 °C after loading Pd. The synthesized 1% Pd/ZnO nanocomposites not only showed the maximum response value 19.20 toward 5000 ppm CH 4 at 200 °C, but also exhibited the excellent selectivity and good repeatability. The improvement of CH 4 sensing performance by Pd nanoparticles could be attributed to the synergy effect with the spill-over effect and the nano-Schottky barriers.

研究领域: 材料科学 · 纳米科技 · 传感器技术 · 表面化学 · 半导体材料
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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Dynamic Modification of Palladium Catalysts with Chain Alkylamines for the Selective Hydrogenation of Alkynes

Qian Luo,Zhe Wang,Yuzhuo Chen,Shanjun Mao,Kejun Wu,Kaichao Zhang,Qichuan Li,Guofeng Lv,Guodong Huang,Haoran Li,Yong Wang

Selective hydrogenation of alkynes plays a pivotal role in the field of chemical production but still suffers from restrained catalytic activity and low alkene selectivity. Herein, a dynamic modification strategy was utilized by preferentially attaching diethylenetriamine (DETA) to the surface of the support to modify the Pd catalyst. The DETA-modified Pd catalyst demonstrates unprecedented reactivity (14,412 h–1) and selectivity as high as 94% for the semihydrogenation of 2-methyl-3-butyn-2-ol at 35 °C, presenting a 36-fold higher reactivity than the Lindlar catalyst. Moreover, the yield exceeds 98.2% at full conversion under no solvent and organic adsorbate conditions, indicating the potential applications for industrial production. Systematic studies reveal that flexible DETA serves in a reversible “breathing pattern” for the molecular discrimination by constructing dynamic metal–support interaction (DMSI), enabling selective exclusion of alkenes from the Pd surface. DETA is competent to dynamically adjust the adsorption behaviors of reactants and effectively boost the intrinsic activity of the modified catalyst. Impressively, the DETA-modified Pd catalyst exhibits exceptional stability even after being recycled 20 times. This work sheds light on a novel and applicable method for the rational design of heterogeneous catalysts via DMSI.

研究领域: 催化化学 · 材料科学 · 工业化学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2025 · IF 8.3

Highly efficient hydrogen getters with enhanced CO resistance via one-step ball milling

Biye Niu,Feixiang Gao,Zekun Jing,Taiping Fu,Yufeng Liu,Yakun Guo,Maobing Shuai

In confined environments, hydrogen accumulation presents significant safety hazards, necessitating the development of efficient hydrogen uptake materials. Conventional Pd/C-DEB hydrogen getter is severely compromised by CO poisoning. This study introduces a one-step mechanochemical ball milling approach that integrates Pd/C catalysts with DEB to fabricate a CO-tolerant hydrogen getter. A DEB conversion rate of 75.2 % is achieved under an H 2 atmosphere containing 1 % CO, representing a sixfold improvement over the untreated sample. Ball milling refines Pd nanoparticles, increases surface area, generates multiscale defects, strengthens metal-support interactions, enhances electron transfer, modulates the Pd d-band structure, and reduces CO adsorption energy, thereby exposing more active sites for hydrogen uptake. This approach is also applicable to Pt/C, Rh/C, and other platinum-group metal systems, providing a versatile strategy for designing durable and CO-resistant getters in energy storage and conversion technologies.

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NANOTECHNOLOGY · 2022 ·Vol. 33 ·期 37 ·375401 · IF 3.953

Tannic acid modified PdAu alloy nanowires as efficient oxygen reduction electrocatalysts

Hongjing Wang,Shiqian Jiao,Songliang Liu,Shuli Yin,Tongqing Zhou,You Xu,Xiaonian Li,Ziqiang Wang,Liang Wang

Design of the structure, composition and interface of the catalysts is very important to improve oxygen reduction reaction (ORR) catalytic activity under alkaline environment. Herein, we propose a direct method to rapid synthesis of tannic acid (TA) modified PdAu alloy nanowires (PdAu@TA NWs). Compared with pure PdAu NWs and commercial Pt/C, the PdAu@TA NWs exhibit superior ORR electrocatalytic activity (mass activity: 0.73 A mg−1metal and specific activity: 3.50 mA cm−2), stability, and methanol tolerance in an alkaline medium because PdAu@TA NWs possess sufficient active sites and synergistic effect that can effectively promote the oxygen reduction, inhibit the oxidation of the catalyst and improve the methanol tolerance of the catalyst. This synthetic method is a promising strategy to prepare metallic catalyst with surface functionalization.

研究领域: 材料科学 · 电化学 · 催化科学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2018 · IF 4.229

PtPd nanoparticles supported on sulfonated nitrogen sulfur co-doped graphene for methanol electro-oxidation

Kangning Zhang,Xiaoling Chen,Lina Wang,Dongxia Zhang,Zhonghua Xue,Xibin Zhou,Xiaoquan Lu

In this paper, sulfonated nitrogen sulfur co-doped graphene (S-NS-GR) nanocomposite , i.e., nitrogen sulfur co-doped graphene functionalized with SO 3 H group as a novel catalyst support material was prepared. Pt Pd nanoparticles (Pt Pd NPs) were deposited on the surface of S-NS-GR by a facile electrochemical approach. The morphology and structure of Pd-PtNPs/S-NS-GR were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), energy dispersive X-ray spectroscopy (EDS) and electrochemical impedance spectroscopy (EIS), respectively. In addition, the electrocatalytic performance of catalyst for methanol oxidation reaction (MOR) was systematically studied by cyclic voltammetry and chronoamperometry in alkaline media . Compared with Pt Pd NPs supported on nitrogen sulfur co-doped graphene (Pt-PdNPs/NS-GR), the excellent performance of Pd-PtNPs/S-NS-GR is mainly ascribed to the embedding of abundant functional groups ( SO 3 H) into the NS-GR layers, which not only facilitate the homogeneous distribution of metal NPs , but also strengthen the interaction between metals and support material, thus improve the stability of catalyst in MOR.

研究领域: 材料科学 · 电化学
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ELECTROCHIMICA ACTA · 2016 · IF 4.803

Improvement of electrochemical reductive dechlorination of 2,4-dichlorophenoxyacetic acid using palladium catalysts prepared by a pulsed electrodeposition method

Zhiqiao He,Qiwei Jian,Juntao Tang,Tao Xu,Jinli Xu,Zhesheng Yu,Jianmeng Chen,Shuang Song

A nickel-foam, supporting palladium particles (PE-Pd/foam-Ni), was fabricated by pulsed electrodeposition. The PE-Pd/foam-Ni was proven to be a promising electrode for electro-catalytic reductive dechlorination of 2,4-dichlorophenoxyacetic acid (2,4-D) in aqueous solution. Compared to the traditional chemical deposition of palladium on a foam-nickel electrode, the PE-Pd/foam-Ni exhibits markedly improved removal efficiency and current efficiency (CE) for the dechlorination of 2,4-D. The PE-Pd/foam-Ni electrode with 0.67   mg Pd loading could achieve a maximum 2,4-D removal efficiency of 98% and a CE of 14% after 3   h at a current density of 1.5   mA   cm −2 . Moreover, the PE-Pd/foam-Ni maintained stable performance throughout three successive recyclability tests. As supported by physical-chemical characterization, the palladium catalysts originated from pulse electrodeposition possess a higher percentage of exposed {111} facets and a higher number of low-coordinated (edge/corner) sites, associated with a smaller particle size, in comparison with catalysts obtained from chemical deposition. Since the palladium atoms located on the edge/corner sites facilitate the catalytic reaction and the exposed {111} facets favor the generation and stabilization of chemisorbed active hydrogen, the enhanced electrocatalytic dechlorination performance of PE-Pd/foam-Ni electrode can be ascribed to the improved intrinsic properties of the Pd catalyst.

研究领域: 环境科学 · 电化学 · 催化材料
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APPLIED SURFACE SCIENCE · 2021 · IF 6.707

Polyethylenimine modified ultrafine palladium nanocrystals on reduced graphene oxide for hexavalent chromium reduction

Yuxin Yin,Jun Hao,Yi Yang,Jun Zhao,Jie Song

Palladium-catalytic hydrogenation is an efficient method for remediating inorganic/organic contaminants. Herein, a very simple adsorption-reduction strategy is applied to synthesize the polyethylenimine (PE) modified ultrafine palladium nanocrystals on reduced graphene oxide (RGO) hybrids (PE@Pd-RGO). The surface composition, structure, and morphology of PE@Pd-RGO hybrids are minutely characterized by various physical characterization techniques and the formation mechanism of PE@Pd-RGO hybrids is defined according to experimental observation. Physical characterizations demonstrate that palladium nanocrystals with only 2.91 nm size uniformly anchor at RGO surface and PE modification endows PE@Pd-RGO hybrids with eminent water-solubility. When applied as catalyst for hexavalent chromium reduction, PE@Pd-RGO hybrids reveal excellent catalytic activity (rate constant: 0.0785 min −1 , turnover frequency: 1.166 mol Cr mol Pd −1 min −1 ) and stability due to the small particle size of palladium nanocrystals, excellent colloidal stability, and distinctive electrostatic attraction between PE with –NH 3 + and Cr 2 O 7 2- ion.

研究领域: 环境科学 · 材料科学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2021 · IF 4.539

Zwitterionic daptomycin stabilized palladium nanoparticles with enhanced peroxidase-like properties for glucose detection

Ying Liang,Hongchen Li,Liyuan Fan,Ruyu Li,Yanshuai Cui,Xianbing Ji,Haiyan Xiao,Jie Hu,Longgang Wang

Mimic enzymes , especially noble metal nanomaterials , replace natural horseradish peroxidase due to the artificial regulation of catalytic activity by adjusting particle size and morphology. However, the existing mimic enzymes still have disadvantages such as large particle size, easy clustering and poor biocompatibility . Herein, well-dispersed daptomycin stabilized palladium nanoparticles (Dap-Pd n NPs) were synthesized by using daptomycin as a biological template . The average particle size of palladium nanoparticles of Dap-Pd 0.25 NPs was 1.73 nm, the hydrodynamic size of Dap-Pd 0.25 NPs detected by DLS method was 49.97 nm, Dap-Pd 0.25 NPs were stable in fibrinogen solution. In addition, Dap-Pd 0.25 NPs had excellent peroxidase-like activity, which effectively catalyzed the colorimetric oxidation reaction of 3,3′,5,5′-tetramethylbenzidine (TMB) by H 2 O 2 . Dap-Pd 0.25 NPs were used to detect glucose concentration based on the colorimetric reaction of TMB, which had a wide detection range (0.02–1 mM) and low detection limit (5.6 μM) for glucose. Besides, fluorescence experiments proved that Dap-Pd n NPs catalyzed H 2 O 2 to generate·OH. Taken together, a simple, green and inexpensive synthesis method of palladium nanoparticles with enhanced peroxidase-like activity was proved in this research. Dap-Pd n NPs will have great application prospects in biological detection in the future.

研究领域: 生物化学 · 纳米医学 · 分析化学
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