Sustainable Energy & Fuels
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2024
·
IF 5
Zhenluo Yuan,Ouyang Liu,Shuyan Guan,Xianyun Liu,Linyan Bian,Qiuming Peng,Shumin Han,Yanping Fan,Baozhong Liu
Formic acid (FA) is a potential hydrogen storage material for hydrogen storage and production under moderate circumstances using a catalytic method. Exploring excellent catalysts to achieve rapid FA dehydrogenation remains a challenge for a low-carbon economy. In this work, a series of PdAg alloys anchored on N-doped carbon dots (CDs) were used for efficient FA dehydrogenation at ambient temperature. The optimized Pd0.9Ag0.1/CDs catalyst can catalyze complete dehydrogenation of FA in 9.5 min with a TOF value of 617 h−1 at 298 K. Experiments reveal that the high activity of FA dehydrogenation is attributed to the electron transfer in PdAg alloys and the strong electronic interaction between PdAg alloys and CDs supports. Furthermore, the CDs support restricts the growth and aggregation of PdAg nanoparticles during the reaction of FA dehydrogenation. This work provides a simple approach to the fabrication of CDs supported highly distributed PdAg alloy catalysts for efficient utilization in the hydrogen energy field.
研究领域:
催化化学
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材料科学
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氢能技术
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DOI
高影响因子
ChemistrySelect
·
2024
·Vol. 9
·期 25
·e202402023
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IF 1.9
Siyi Zeng,Haonan Li,Qian Zhang,Xiangyi Gong,Shaohua Jin,Chongchong She,Junfeng Wang,Lijie Li,Kun Chen,Guanghui Wang
Graphical Uniformly loaded PdAg bimetallic catalysts were synthesized by chemical reduction method to investigate the effects of different Pd/Ag ratios and catalysts with different carriers on the activity of hydrogen production by formic acid decomposition. The catalysts were tested at different reaction temperatures. Hydrogen (H 2 ) is recognized as a clean energy carrier with great potential for the future energy systems. Given the existing challenges in direct H 2 storage and delivery, the current option for utilizing hydrogen energy is to produce hydrogen from its storage carriers on-site, and the development of a highly active, highly selective, and highly stable catalyst for H 2 production is an important part of this. Herein, PdAg alloy was deposited on mesoporous carbon nitride (mpg-C 3 N 4 ) as a catalyst for the dehydrogenation of the formic acid (FA). The synergistic effect of Pd and Ag metals for catalysis was explored. The role of the supports on the catalytic performance was also demonstrated by depositing PdAg alloy on several carriers of Silica@Resorcinol-Formaldehyde Spheres, Carbon Flower Particles and SBA-15. Pd 1 Ag 1/2 / mpg -C 3 N 4 showed a considerable activity during FA dehydrogenation with a turnover frequency (TOF) value of 887 h −1 at 333 K, demonstrating that carbon nitride as a carrier has a significant enhancement on the catalytic hydrogen production from formic acid.
研究领域:
化学工程
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材料科学
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能源科学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
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IF 7.489
Xiaomin Meng,Yirui Ouyang,Huijie Wu,Haowei Huang,Fengqian Wang,Shuo Wang,Mengchao Jiang,Lian Ying Zhang
Tuning the chemical composition and surface structure of electrodes is demonstrated as a feasible and effective strategy to tailor advanced catalysts for energy electrocatalysis. In this work, hierarchical palladium-silver alloy nanosheets (PdAg NS) with the thickness ~7 atoms and rich atomic defects are successfully prepared, using the carbon monoxide (CO) confinement approach. The optimized Pd 7 Ag 3 NS/C exhibits 8.8 times higher catalytic peak current density and much better stability toward ethanol electrooxidation than Pd NS/C catalyst. The catalytic enhancement mechanism could be attributed to the synergetic effects among optimized electronic structure of Pd, novel architecture, and rich atomic defects.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2020
·Vol. 2021
·期 2
·156-165
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IF 2.529
Gongguo Zhang,Yanyun Ma,Feng Liu,Xiaowei Fu,Xiaoqian Luan,Fengli Qu,Maochang Liu,Yiqun Zheng
Graphical Gold@palladium-silver alloy core-shell dendritic nanocrystals with tunable size and elemental composition were fabricated in high purity via seeded growth. Compared to commercial Pd/C catalysts, the current products exhibit enhanced activity and excellent operation stability for electroxidation of ethanol in alkaline media. We report a facile synthesis of Au@PdAg alloy core-shell nanocrystals in dendrite form, having tunable size and composition. In particular, using spherical Au nanoparticles as seeds, the co-reduction of Pd and Ag precursor in growth stage results in the formation of PdAg alloy shells with a dendrite shape. Their size and elemental composition can be tuned by varying the seed amount and feeding ratio in Pd and Ag precursor, respectively, illustrating the versatility of the current synthetic strategy. The size, morphology, and elemental composition of the products have been characterized using a set of techniques, including SEM, TEM, XRD, XPS, HAADF-STEM, and EDX-STEM mapping. When working as electrocatalysts, the current Au@PdAg alloy core-shell nanocrystals supported by carbon black exhibit enhanced activity and excellent operation stability for electroxidation of ethanol as compared to commercial Pd/C. The current work offers a feasible strategy to preparation of multi-metallic core-shell dendritic nanocrystals with controllable size and composition and could find important use in fuel cells and related fields.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Rongrong Li,Wubing Yao,Yanxian Jin,Wenping Jia,Xiaoying Chen,Jingjing Chen,Jianli Zheng,Yuan Hu,Deman Han,Jia Zhao
Hydrocinnamaldehyde (HCAL) is a crucial intermediate in the manufacture of perfumes and pharmaceuticals, but highly selective hydrogenation of cinnamaldehyde (CALD) to hydrocinnamaldehyde with a good conversion rate is a challenging. We report that the incorporation of Ag into Pd-based catalysts promotes their catalytic activity and HCAL selectivity (HCAL selectivity of 98.6% with >99.9% CALD conversion for Pd-0.3Ag/MCM-41) for CALD hydrogenation compared to those of catalysts with no Ag, e.g., HCAL selectivity of 84.5% for Pd/MCM-41and 77.3% for Pd/AC (activated carbon). The Pd-0.3Ag/MCM-41 catalyst shows an outstanding stability during five cycles of use. The excellent performance of the Pd-0.3Ag/MCM-41 catalyst in CALD hydrogenation is due to the ultra-small size of the Pd nanoparticles (Pd-Ag alloy, a geometric and electronic modification of Pd).
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
RENEWABLE ENERGY
·
2023
·
IF 8.7
Qunying Sun,Huanhuan Zhang,Yanping Fan,Linyan Bian,Qiuming Peng,Baozhong Liu
Regulating the electronic structure of noble metals through metal alloy–support interactions is significant for hydrogen economy . Herein, a PdAg alloy highly dispersed on the surface of Ti 3 C 2 is successfully designed through a simple microwave-assisted reduction method. The catalytic activity of PdAg alloys with various molar ratios manifests obviously enhanced catalytic activity compared to monometallic catalysts toward hydrogen generation in ammonia borane (AB) hydrolysis. Specifically, Pd 4 Ag 1 /Ti 3 C 2 presents an optimal turnover frequency (TOF) value of 1296 min− 1 at room temperature and a lower activation energy ( E a ) of 38.8 kJ mol -1 . Through the experimental results, the formation of a PdAg alloy with the introduction of the second metal Ag adjusts the electronic structure around Pd and enhances the catalytic activity. Additionally, the metal alloy–support interaction between Ti 3 C 2 and the PdAg alloy significantly promotes hydrogen generation during the hydrolysis of AB. This study provides new ideas and a reasonable basis for heterogeneous catalysis based on bimetallic catalysts .
研究领域:
催化化学
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材料科学
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氢能技术
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产品关联
DOI
高影响因子
CATALYSIS LETTERS
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2020
·Vol. 151
·期 6
·1796-1804
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IF 2.482
Wang Haiyan,Zhang Yating,Yan Fangfang,Zhang Hucheng
Abstract The biorenewable alcohols are identified as the promising energy in fuel cells, but the lack of efficient catalysts limits the electricity output. Here, we chemically grew the PdAg alloy nanoparticles (NPs) on reduced graphene oxide (RGO) to obtain Pd x Ag y (m)/RGO, and investigated the dependences of peak current densities on the metal loadings (m), Pd mole fractions (x), and sizes. The maximal peak currents of 1.86, 4.88, 14.3 and 13.6 × 10 4 mA cm −2 mg Pd −1 were respectively achieved in the electrooxidation reactions of methanol, ethanol, ethylene glycol and glycerol. It is shown that the interactions of PdAg NPs with RGO can control the catalytic efficiencies through mediating the electronic characteristics of metal NPs and the reactant absorptions. Except the catalysts for methanol oxidation reaction, the efficient catalysis possesses the same lattice structure in PdAg alloys with the optimized m, and gives a common descriptor to select the catalyst with high catalytic activity. Graph Abstarct
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
·
2015
·Vol. 3
·期 31
·15920-15926
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IF 7.443
Pei Song,Jiu-Ju Feng,Fei-Ying Guo,Ai-Jun Wang
In this work, porous bimetallic palladium–silver (Pd63Ag37) alloy nanocorals were synthesized by a simple and facile one-pot polyol method. The composition and morphology of the nanocrystals were well controlled by changing the concentrations of the precursors. The obtained nanocrystals were mainly characterized by scanning electron microscopy, transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and the Brunauer–Emmett–Teller method. Porous Pd63Ag37 nanocorals had an enlarged electrochemically active surface area (55.85 m2 g−1), and exhibited enhanced electrocatalytic activity and improved stability for glycerol oxidation reaction as compared to commercial Pd black, owing to the unique porous coral-like nanostructures and synergistic interactions of the alloyed bimetals.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
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2024
·Vol. 121
·期 17
·e2318853121
·
IF 9.4
Junliang Chen,Fangzhou Zhang,Min Kuang,Li Wang,Huaping Wang,Wei Li,Jianping Yang
Recently, there has been a notable surge in interest regarding reclaiming valuable chemicals from waste plastics. However, the energy-intensive conventional thermal catalysis does not align with the concept of sustainable development. Herein, we report a sustainable electrocatalytic approach allowing the selective synthesis of glycolic acid (GA) from waste polyethylene terephthalate (PET) over a Pd67Ag33 alloy catalyst under ambient conditions. Notably, Pd67Ag33 delivers a high mass activity of 9.7 A mgPd−1 for ethylene glycol oxidation reaction (EGOR) and GA Faradaic efficiency of 92.7 %, representing the most active catalyst for selective GA synthesis. In situ experiments and computational simulations uncover that ligand effect induced by Ag incorporation enhances the GA selectivity by facilitating carbonyl intermediates desorption, while the lattice mismatch-triggered tensile strain optimizes the adsorption of *OH species to boost reaction kinetics. This work unveils the synergistic of strain and ligand effect in alloy catalyst and provides guidance for the design of future catalysts for PET upcycling. We further investigate the versatility of Pd67Ag33 catalyst on CO2 reduction reaction (CO2RR) and assemble EGOR//CO2RR integrated electrolyzer, presenting a pioneering demonstration for reforming waste carbon resource (i.e., PET and CO2) into high-value chemicals.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
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