JOURNAL OF POWER SOURCES
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2012
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IF 4.951
Haiting Lu,Yang Fan,Ping Huang,Dongli Xu
SnO 2 nanospheres were employed as the support material for Pd catalyst. The as-prepared Pd/SnO 2 catalyst exhibited remarkably improved electrocatalytic activity and stability towards formic acid oxidation , in comparison with that of the Vulcan XC-72 carbon black and the commercial SnO 2 nanopowder supported Pd catalyst. The enhanced catalytic performance may arise from the unique structure and surface properties of the SnO 2 nanospheres, which process extraordinary promotional effect on Pd catalyst.
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CHEMOSPHERE
·
2015
·
IF 3.34
Ya-Li Chen,Lu Xiong,Xiang-Ning Song,Wei-Kang Wang,Yu-Xi Huang,Han-Qing Yu
Electrocatalytic hydrodehalogenation is a cost-effective approach to degrade halogenated organic pollutants in groundwater, and Pd-based catalysts have been found to be an efficient cathode material for this purpose. In this work, a novel Cu@Pd bimetallic catalyst loaded on Ti plate was prepared via combined electrodeposition and galvanic replacement for electrocatalytic hydrodehalogenation of atrazine, a typical halogenated pollutant. The obtained bimetallic catalyst with uniformly dispersed Pd nanoparticles possessed a large electrochemically active surface area of 572 cm 2 . The Cu@Pd/Ti cathode exhibited a higher electrocatalytic efficiency towards atrazine reduction than the individual Pd/Ti or Cu/Ti cathodes, and achieved up to 91.5% within 120 min under a current density of 1 mA cm −2 . Such an electrocatalytic reduction followed pseudo-first-order kinetics with a rate constant of 0.0214 min −1 . Atrazine was selectively transformed to dechlorinated atrazine, and its degradation pathway was identified. Current density was found to have a critical influence on the atrazine reduction due to the competitive hydrogen evolution reaction at a higher current density. The fabricated bimetallic catalyst also exhibited a good stability. This work provides an efficient and stable electrocatalyst for chlorinated contaminate removal and groundwater remediation.
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Interdisciplinary Materials
·
2024
·
IF 24.5
Mingwei Wang,Zhiyi Hu,Jieheng Lv,Zhiwen Yin,Zhewei Xu,Jingfeng Liu,Shihao Feng,Xiaoqian Wang,Jiazhen He,Sicheng Luo,Dafu Zhao,Hang Li,Xuemin Luo,Qi Liu,Damin Liu,Baolian Su,Dongyuan Zhao,Yong Liu
Compositions and morphologies of Pt-based electrocatalysts have great impact on the electrocatalytic activity and stability of oxygen reduction reaction (ORR). Herein, we report a novel design of one-dimensional (1D) Pt–Pd dendritic nanotubular heterostructures (DTHs) by controlling the degree of Pt 2+ -Pt reduction reaction and Pd-Pt galvanic replacement reaction with uniform Pd nanowires as sacrificial templates. The obtained Pt–Pd bimetallic DTHs catalyst exhibited uniform and dense Pt dendritic nanobranches on the surface of 1D hollow Pt–Pd alloy nanotubes, possessing superior catalytic activity for ORR compared to state-of-the-art commercial Pt/C catalysts. Typically, the Pt 4 Pd DTHs catalyst showed efficient mass activity (MA, 1.05 A mg Pt −1 ) and specific activity (SA, 1.25 mA cm Pt −2 ) at 0.9 V (vs. RHE), and the catalyst exhibited high stability with 90.4% MA retention after 20 000 potential cycles. The Pt–Pd bimetallic DTHs configuration combines the advantages of 1D hollow nanostructures and dense Pt dendritic nanobranches, which results in rich electrochemical active surface sites, fast charge transport, and multiple dendritic anchoring points contact on carbon support, thus boosting its catalytic activity and stability towards electrocatalysis.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2016
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IF 3.014
Xiaomeng Li,Ming Wen,Dandan Wu,Qingsheng Wu,Jiaqi Li
For the exploration of catalysts with excellent performance in alkaline fuel cells, high-performance two-dimensional (2D) Pd-on-NiCu nanosheets were synthesized through the kinetics controlling synthesis of NiCu nanosheets followed by Pd nanoparticles (NPs) embedding treatment at room temperature. In which case, well-dispersed Pd NPs with the average diameter of ∼4 nm are embedded on NiCu nanosheets (BET surface area of 180.7 m 2 g −1 ). Pd-on-NiCu nanosheets exert remarkable high performance in electrocatalytic activity, methanol-tolerance and stability, the electrocatalytic mass activity of Pd-on-NiCu nanosheets is 1827 mAmg −1 , which is over 6-fold higher than that of commercial Pd/C (289 mAmg −1 ), and the current density of the electrocatalyst decreases after 300 cycles of only 6%. Therefore, Pd-on-NiCu nanosheets can be considered as one of the most promising candidates for fuel cells applications.
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CATALYSIS LETTERS
·
2017
·Vol. 147
·期 7
·1802-1810
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IF 2.799
Hong Runrun,He Yufei,Miao Chenglin,Feng Junting,Li Dianqing
Abstract Pd–Ir mesocrystals with rough surface and highly branched structure were synthesized through a facile co-reduction method. The morphology evolution shows the mesocrystals were formed by oriented attachment of nanoparticles, and abundant defects sites as well as synergetic effect between building units were formed during mesocrystals oriented attachment process. Therefore, the supported Pd–Ir mesocrystals show a significant enhancement in catalytic performance in hydrogenation of 2-ethylanthraquinone compared with conventional Pd–Ir nanoparticles. The high activity can be ascribed to high densities of defect sites in Pd–Ir MCs catalyst, which facilitated H 2 activation. In addition, the geometric effect of Pd–Ir MCs catalyst was responsible for inhibiting further hydrogenation of eAQH 2 to undesired consecutive byproducts. Graphical Abstract
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Scientific Reports
·
2017
·Vol. 7
·期 1
·1-9
·
IF 4.259
Qu Qing,Zhang Jian-Hua,Wang Jing,Li Qing-Yu,Xu Chang-Wei,Lu Xihong
Considerable efforts have been devoted recently to design and fabrication of high performance and low cost electrocatalysts for oxygen evolution reaction (OER). However, catalytic activity of current electrocatalysts is usually restricted by high onset potential and limited active sites. Herein, we fabricated three-dimensional (3D) highly ordered mesoporous Pd-Co 3 O 4 composite materials as excellent electrocatalysts for OER in alkaline solution with high activity and stability. Three-dimensional highly ordered mesoporous Co 3 O 4 material was firstly synthesized using mesoporous silica KIT-6 as hard template. Then, Pd-Co 3 O 4 nanomaterials were prepared by a simple reduction method. The as-prepared 3D mesoporous Pd-Co 3 O 4 catalysts have ordered mesoporous structure with a high surface area of 81.0 m 2 g −1 . Three-dimensional highly ordered mesoporous structure can facilitate diffusion and penetration of electrolyte and oxygen. Moreover, the catalysts can also keep catalyst particles in a well dispersed condition with more catalytic active sites. Electrochemical measurements reveal that the 3D mesoporous Pd-Co 3 O 4 catalysts exhibit superior performance in alkaline solution with low onset potential (0.415 V vs . SCE) and excellent long-duration cycling stability.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2016
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IF 3.205
Qizhi Dong,Meiling Huang,Cancheng Guo,Gang Yu,Mimi Wu
There is significant interest in developing new catalyst supports such as metal carbides to overcome the electrochemical corrosion problem of traditional high surface area carbon. A key challenge is the dispersion and stability of the catalysts on the non-carbon based materials. This paper reports a new approach to functionalize titanium carbide by poly (diallyldimethylammonium chloride) (PDDA), investigated as a new catalyst support for Pd catalyzed electrochemical reaction . Thermal gravimetric analysis confirmed the successful noncovalent functionalization of TiC by PDDA. Pd nanoparticles are deposited in situ on the PDDA-wrapped TiC surface through electrostatic interactions mechanism. According to transmission electron microscopy (TEM) observations, Pd nanoparticles with a mean size of ∼2.9 nm are homogeneously deposited on TiC(P). Among all the samples tested, the Pd/TiC(P) catalysts exhibit the highest resistance to CO poisoning, catalytic activity and stability towards formic acid electrooxidation . This performance was attributed to a strong Pd↔TiC interaction and the formation of oxygenated species on the TiC.
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APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING
·
2015
·Vol. 119
·期 2
·603-608
·
IF 1.704
Zhang Yulong,Xu Zhizhen,Sun Huanghui,Qiu Qiaoli,Zhang Lingfan,Xia Wei,Zhang Wenqing
In this study, we have constructed nano-sized hollow carbon spheres with large cavities and thin shells under hydrothermal conditions using ricinoleic acid as the soft template and 2,4-dihydroxybenzoic acid and hexamethylenetetramine as the sphere precursors. After being filled with Fe particles and loaded with Pd particles, the spheres became magnetic, allowing easy separation from the liquid phase by a magnet, and showed excellent catalytic performance in decomposing formic acid. The hollow carbon spheres and the magnetic catalysts were characterized by TEM, FE-SEM, XPS, and FTIR.
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CATALYSIS LETTERS
·
2024
·
IF 2.3
Zhao Chunzhi,Mao Dongsen,Meng Tao,Guo Qiangsheng,Yu Jun
Owing to the intrinsic nature of the uniformed topologies and ultrasmall Zr 6 nodes of Zr-MOFs, herein, we employed Zr-MOFs (UiO-66 and UiO-67), as opposed to the support of traditional ZrO 2 , to prepare the Pd catalysts for toluene degradation. Compared with the catalysts of Pd/UiO-66 and Pd/ZrO 2 , Pd/UiO-67 catalyst boosted an excellence catalytic performance for toluene degradation, giving the lowest T 90% value of 235 °C with long-term stability. With the assisting of the cavity confinement of Zr-MOFs, Pd nanoparticles are prone to be encapsulated in the 3D frameworks of Zr-MOFs, and the bigger micropores of UiO-67 are more conducive to the formation of larger Pd nanoparticles. The in situ FT-IR results further declared that although the active sites are partly sacrificed due to the larger Pd nanoparticles formed in UiO-67, the stable adsorbed toluene on Pd/UiO-67 boosted the quick degradation of toluene in the reaction interval even without undergoing intermediate processes of benzoate and benzaldehyde. Graphical Abstract UiO-66, UiO-67 and ZrO 2 were employed to prepare the Pd catalysts for toluene degradation, Pd/UiO-67 catalyst boosted an excellence catalytic performance with long-term stability.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-11
·
IF 14.7
Pei An,Wang Peng,Zhang Shiyi,Zhang Qinghua,Jiang Xiaoyi,Chen Zhaoxi,Zhou Weiwei,Qin Qizhen,Liu Renfeng,Du Ruian,Li Zhengjian,Qiu Yongcai,Yan Keyou,Gu Lin,Ye Jinyu,Waterhouse Geoffrey I. N.,Huang Wei-Hsiang,Chen Chi-Liang,Zhao Yun,Chen Guangxu
Challenges in direct catalytic oxidation of biomass-derived aldehyde and alcohol into acid with high activity and selectivity hinder the widespread biomass application. Herein, we demonstrate that a Pd/Ni(OH) 2 catalyst with abundant Ni 2+ -O-Pd interfaces allows electrooxidation of 5-hydroxymethylfurfural to 2, 5-furandicarboxylic acid with a selectivity near 100 % and 2, 5-furandicarboxylic acid yield of 97.3% at 0.6 volts (versus a reversible hydrogen electrode) in 1 M KOH electrolyte under ambient conditions. The rate-determining step of the intermediate oxidation of 5-hydroxymethyl-2-furancarboxylic acid is promoted by the increased OH species and low C–H activation energy barrier at Ni 2+ -O-Pd interfaces. Further, the Ni 2+ -O-Pd interfaces prevent the agglomeration of Pd nanoparticles during the reaction, greatly improving the stability of the catalyst. In this work, Pd/Ni(OH) 2 catalyst can achieve 100% 5-hydroxymethylfurfural conversion and >90% 2, 5-furandicarboxylic acid selectivity in a flow-cell and work stably over 200 h under a fixed cell voltage of 0.85 V.
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Molecular Catalysis
·
2024
·
IF 3.9
Xiaoying Zhou,Shiyu Fang,Zihao Hu,Zuliang Wu,Jing Li,Wei Wang,Jiali Zhu,Shuiliang Yao,Erhao Gao
This study introduces a novel catalyst system comprising Pd nanoparticles loaded onto Mn-doped NiO for the efficient oxidation of methane (CH 4 ) at low temperatures. The loading of Pd nanoparticles onto the Mn-doped support has yielded a catalyst with exceptional activity and stability, as evidenced by the lowest T 50 temperature of 276 °C and a CH 4 conversion reaching 97% at 325 °C. The catalyst demonstrates optimized reaction kinetics with the lowest activation energy of 69.2 kJ mol –1 . The catalyst's superior performance is attributed to the synergistic effects of the Pd/Mn-NiO composite, which include a higher Pd 2+ /Pd 4+ ratio, increased adsorptive oxygen concentration (O ads /O total ), and a reduced Ni 3+ /Ni 2+ ratio. These characteristics collectively enhance the catalytic activity for CH 4 oxidation. The Mars-van Krevelen mechanism underpins the oxidation process, with Pd 2+ identified as the principal active site for CH 4 adsorption and dissociation. Diffuse reflectance infrared Fourier transform spectroscopy coupled with mass spectrometry elucidates the pathway of surface reactive oxygen species in the formation of key intermediates, such as formates, and underscores the accelerated decomposition of carbonate facilitated by the Pd modification on the Mn-NiO surface. The findings signify a significant advancement in the development of catalysts for environmental and energy-related applications, particularly in the mitigation of CH 4 emissions.
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JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Wei Jia,Wengang Liu,Yuandong Cui,Hang Song,Chengfeng Zhou,Wei Jiang,Haoxi Ben,Xiaoli Yang,De Chen
Converting cellulose into C 2 alcohols presents a sustainable alternative to fossil fuels, contributing to the development of eco-friendly and economically viable biofuels and chemicals. Tungsten oxide (WO 3 ) is a key solid acid catalyst for this process, yet limited research explores its diverse morphologies and unique catalytic effects. This study investigates diverse WO 3 morphologies (nanosheets, nanoflowers, nanoblocks, and tetrahedral octahedra) in combination with Pd for converting cellulose to C 2 alcohols. Optimized conditions with Pd/o-WO 3 catalyst resulted in the highest C 2 alcohols (ethylene glycol and ethanol, 80.9 %), notably yielding 64.8 % ethylene glycol. Extensive characterizations and DFT calculations reveal the smaller element occupancy rates and a longer W-O bond length led to a large number of crystal defects over Pd/o-WO 3 . It facilitated the formation of W 5+ –OH sites and Pd-O(H)-W interactions, further synergistically enhancing hydrogenation ability and acidity. Designed experiments to elucidate cellulose conversion pathways, including hydrolysis, retro -aldol condensation, and hydrogenation. This study emphasizes the unique impact of WO 3 morphologies and underscores the importance of supporting crystal defects for catalytic performance in eco-friendly biofuel and chemical production.
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