APPLIED CATALYSIS A-GENERAL
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2019
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IF 4.63
Yuhai Sun,Jingjing Li,Peirong Chen,Bangfen Wang,Junliang Wu,Mingli Fu,Limin Chen,Daiqi Ye
Palladium-loaded ZnO (Pd/ZnO) catalyst was synthesized by co-precipitation method and evaluated for plasma-catalytic reverse water-gas shift (RWGS) reaction. A CO 2 conversion of 32.5 % was achieved on “Pd/ZnO + Plasma”, and was around two times higher than that of “ZnO + Plasma” (17.3 %). Catalyst characterization by X-ray diffraction, high-resolution transmission electron microscopy, temperature-programmed reduction and quasi in situ X-ray photoelectron spectroscopy revealed the possible formation of ZnO x @PdZn (ZnO x decorated PdZn alloy) at the interface of Pd active phase and ZnO support. The role of ZnO x @PdZn in plasma-catalytic CO 2 conversion was systematically investigated by plasma-excited CO 2 temperature-programmed desorption and in situ Fourier transform infrared spectroscopy. It was found that ZnO x @PdZn at Pd-ZnO interface improved significantly plasma-catalytic CO 2 conversion by promoting the production of bidentate carbonate and bidentate formate species. In situ Raman spectroscopy studies proved that the ZnO x @PdZn remained largely intact during the RWGS process. Our in situ spectroscopic findings thus unveil that the ZnO x @PdZn at Pd-ZnO interface favors the activation of CO 2 , and, consequently, leads to a higher plasma-catalytic performance for CO 2 conversion.
研究领域:
化学工程
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材料科学
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环境科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Shaoda Huang,Shuanglong Lu,Hongyin Hu,Fangping Xu,Huining Li,Fang Duan,Han Zhu,Hongwei Gu,Mingliang Du
Although attentions have been devoted to developing Pd-based bimetallic nanocrystals towards the electrocatalytic oxygen reduction reaction (ORR) and ethanol oxidation reaction (EOR), the engineering of efficient bifunctional electrocatalysts with high atomic utilization still faces big challenges. Herein, we reported a facile one-pot template-free route to fabricate three-dimension hyper-dendritic PdZn nanocrystals (HD-PdZn NCs) that regulated by gas mixtures of carbon monoxide and hydrogen. The developed catalysts acted as robust bifunctional electrocatalysts for cathodic ORR and anodic EOR. Specifically, the engineered HD-PdZn NCs not only displayed superior mass activity (MA, 0.461 A mg Pd -1 ) and specific activity (SA, 0.393 mA cm −2 ) at 0.9 V, which were 5.2 and 5.0 times of commercial Pt/C, respectively, but also showed enhanced stability with only 3% loss of MA after 10,000 cycles for ORR. Density functional theory (DFT) calculations revealed the Zn implantation could facilitate the reduction of OOH* to OH* on the surface of Pd during the ORR process. Moreover, HD-PdZn NCs exhibited the highest EOR mass activity with a value of 3.45 A mg Pd −1 among benchmarked catalysts in alkaline solution. The advantageous structural features and electron effects are proposed to be responsible for the remarkable bifunctional activities. This work illustrates a facile method to fabricate highly efficient bifunctional electrocatalyst for energy conversation application.
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
BIORESOURCE TECHNOLOGY
·
2026
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IF 8.2
Zuhang Jin,Yiwei Zhao,Cheng Tao,Rui Du,Yongzheng Shi,Chao Zhang
PdZn/Mo-Al 2 O 3 -C effectively catalyzed hydrodeoxygenation (HDO) of fatty acid esters to alkanes. • Coexistence of Pd and Zn enhanced the dispersion of active sites and regulates the distribution of acid sites. • ZnO x and MoO x species adjacent to Pd suppressed the decarboxylation side reaction. • 92% octadecane selectivity was achieved in methyl stearate HDO. The conversion of fatty acid esters to alkanes with high carbon chain number by hydrodeoxygenation (HDO) is of great significance in biomass conversion to fuels and chemicals. A PdZn/Mo-Al 2 O 3 -C catalyst was prepared for the preparation of octadecane from methyl stearate HDO. The coexistence of Pd and Zn on Mo-based catalysts greatly promoted the dispersion of active sites on the catalyst surface, which also effectively regulated the distribution of acid sites on the catalyst surface. The Zn modified Pd catalyst also effectively adsorbed the C O/C–O bond of the substrate to facilitate the cleavage of C–O bonds, as well as suppressing the decarboxylation side reaction, and achieving octadecane selectivity of 92%. The optimized catalyst also displayed high HDO selectivity for converting the fatty acid esters (C 8 ∼ C 18 ) to alkanes. Download: Download high-res image (166KB) Download: Download full-size image
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DOI
高影响因子
Molecular Catalysis
·
2023
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IF 4.6
Jihong Jiang,Yongqiang Fang,Yiming Zhao,Lianhua Zhao,Biyao Jin
PdZn intermetallic has excellent electrocatalytic properties due to the strong synergistic effects caused by the ordered arrangement of atoms. It is often synthesized by annealing Pd/ZnO in a hydrogen atmosphere. However, the low conductivity of ZnO crystals limits electron conduction , which is not conducive to electrocatalytic reactions . To avoid conductivity degradation, we annealed Zn 2+ -doped ZIF-67 adsorbed with Pd precursors in a nitrogen atmosphere. The key component, “ghost ZnO,” produced by the decomposition of ZIF during pyrolysis , was used to form intermetallic with Pd by reactive metal-support interaction. The remaining ZnO crystals were converted to amorphous ZnO or removed by sublimation. A composite structure of metal core-intermetallic shell was formed with the surface energy as the driving force. Co@o-PdZn/NC (Pd weight = 2.47 %) exhibited strong oxygen reduction reaction (ORR)/oxygen evolution reaction (OER) electrocatalytic activity (reversible oxygen overpotential of 0.771 V). Moreover, it provided great performance in rechargeable zinc-air batteries (ZABs). In this study, the reactive metal-support interaction (RMSI) between the key component “ghost ZnO” and Pd was used by a one-step annealing method, and the growth process of nanoparticles was precisely controlled using the difference in surface energy between the metals to properly design the catalyst surface structure. The synthesized metal core-PdZn intermetallic shell composite is a promising bifunctional oxygen electrocatalyst . These findings provide a new strategy for designing composites with a metal core-intermetallic shell structure.
研究领域:
材料科学
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电化学
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DOI
高影响因子
Journal of Materials Chemistry A
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2020
·Vol. 8
·期 40
·21327-21338
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IF 11.301
Min Bao,Xinghua Chen,Shiyu Hu,Linqun Zhang,Ying Li,Carlo Carraro,Roya Maboudian,Wei Wei,Yuanjian Zhang,Songqin Liu
In this work, a dual catalyst composed of atomically ordered intermetallic PdZn and Co nanoparticles was synthesized and chemically bonded to nitrogen-doped carbon by simultaneously modulating the lattice spacing of the Pd nanoparticle guest and the metal centers of the zeolite imidazolate framework (ZIF) host through a one-step heating procedure. Results reveal that the ability of the PdZn alloy to catalyze the oxygen reduction reaction can be regulated by adjusting the lattice spacing of Pd–Pd through the formation of the ordered PdZn, resulting from Zn2+ in the ZIF-8 host lattice diffusing into the Pd phase. Meanwhile, the secondary active sites (Co nanoparticles) and N-doped carbon (particularly N-doped carbon nanotubes) carrier are obtained by doping Co2+ into the ZIF-8 host lattice, which can further improve the catalytic activity. The characterization results show the existence of Pd–N and Co–N bonds between the dual catalyst and the carrier, which can be regulated by controlling the synthesis conditions, such as the atomic ratios of the Pd guest to Zn in the ZIF-8 host, pyrolysis temperatures, and doping Co2+ into the ZIF-8 host lattice. The dual catalyst bonded to N-doped carbon exhibits high ORR catalytic activity with a desirable onset potential (0.916 V), and diffusion-limiting current density (∼5.70 mA cm−2), superior to other reported Pd-based catalysts and comparable to commercial Pt/C. Moreover, the chemical bonds between the dual catalyst and the carrier result in the dual catalyst with a small size of 5.9 nm and prolonged duration of electrochemical activity (no obvious change of the half peak potential after 10 000 cyclic voltammetry cycles and 90.6% current retention after a 4 h chronoamperometric test). Thus, the highly dispersed ordered-PdZn/Co on N-doped carbon is a promising substitute to commercial Pt/C for alkaline fuel cells.
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DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
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2025
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IF 4.3
Xing Yan,Dongren Cai,Meihong Lin,Zhijie Wu,Yegang Xia,Yanmei Cai,Sajid Ali,Kok Bing Tan,Andriambinintsoa Ranaivoson Tojonirina,Hao Sun,Guowu Zhan
The selective hydrogenation of CO 2 to methanol demands precise control of both catalyst architecture and reaction pathways. Here, we design an atomic layer deposition (ALD)-engineered Pd/ZnO/ZrO 2 ternary catalyst with atomic-scale ZnO interlayers to decouple and reconfigure active sites at dual interfaces (Pd-ZnO and ZnO-ZrO 2 ). This interfacial engineering drives a 7-fold enhancement in methanol space–time yield (0.584 vs. 0.084 g MeOH g cat −1 h −1 ) and switches the dominant reaction pathway from CO-mediated to formate-driven selectivity (methanol selectivity remarkably surges from 6 % to 64 %). Multimodal characterization and theoretical calculations reveal that ZnO interlayers orchestrate bifunctional cooperation: activating CO 2 /CO adsorption while suppressing CO/CH 4 formation through electronic effects. Long-term stability study uncovers a dynamic restructuring mechanism, where Pd-ZnO interfaces gradually evolve into PdZn β alloy phases under the reaction conditions. This work establishes ALD-mediated interface design as a generalizable strategy to manipulate reaction networks and methanol selectivity in catalytic CO 2 hydrogenation systems.
研究领域:
催化化学
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材料科学
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化学工程
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可持续能源
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表面科学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）