INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2018
·
IF 4.229
Qing Qu,Guo-Liang Pan,Yan-Ting Lin,Chang-Wei Xu
High efficient and low-cost electrocatalysts for the oxygen evolution reaction (OER) are essential components of renewable energy technologies . However, the high onset potential and limited active sites restrict the catalytic activity of current electrocatalysts. Therefore, we are motivated by the development of cheap and efficient catalytic electrodes to promote the sluggish water-splitting systems associated with the large-scale application of clean and renewable energy technologies. Herein, a novel, simple, and efficient routine is presented by noble metal particles embedded within mesoporous metal oxide materials as high-efficiency anode catalysts for OER. Highly ordered mesoporous Co 3 O 4 was prepared by a nanocasting method using the silica KIT-6 as hard template, showing an enhanced electrochemical performance. Then, M - Co 3 O 4 (M = Pt, Pd, Au) nanomaterials were prepared by a simple but novel chemical reduction method. They show the high surface area of 112.3, 81.0 and 73.6 m 2 g −1 , which can provide more active surface area exposure leads to shorter paths of charges from electrolyte to electrode surface . Moreover, a three-dimensional highly ordered mesoporous structure can facilitate diffusion and penetration of electrolyte and oxygen, and can also keep catalyst nanoparticles in a well-dispersed condition with more active sites. Electrochemical measurements revealed that 20, 50, 25 wt% are the best weight contents for M (M = Pt, Pd, Au) in the Co 3 O 4 with highest electrochemical activity (0.410, 0.415 and 0.422 V vs. SCE) and j 0.7V reaching a maximum value. M-Co 3 O 4 (M = Pt, Pd, Au) materials exhibit superior activities and excellent long-duration stability in alkaline attributed to accelerating the formation of Co(IV) cations after being introduced M(M = Pt, Pd, Au) nanoparticles within mesoporous Co 3 O 4 . This kind of noble metal embedded within mesoporous oxide catalysts will hold a large potential as a highly promising electrocatalyst in the future.
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高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Shiqi Peng,Rong Li,Yu Huang,Yufei Zhang,Jun-ji Cao,Shuncheng Lee
Producing the strong metal-support interaction (SMSI) interface and highly reactive oxygen species is a great challenge for catalytic oxidation of formaldehyde (HCHO) at room temperature over supported metal catalysts. Herein, we report a conceptual oxygen vacancy ( V O ) associated SMSI interface of Pt-ZrO 2 nanoparticles for HCHO catalysis at room temperature, exhibiting interfacial dependent reactive oxygen species (O*) formation. The V O on the ZrO 2 support captures and activates the molecular O 2 , then proceeds to generating the reactive oxygen atom (O*) with a lower activation barrier of 0.3 eV. The generated O* tends to link the (1 1 0) surface of ZrO 2 and the (1 1 1) surface of Pt as an electronic transmission channel for the selective catalytic oxidation of HCHO adsorbed on the (1 1 0) surface of ZrO 2 , accelerating the direct generation of formate species and mineralization of HCHO. The Pt- V O -ZrO 2 achieves high HCHO removal and HCHO conversion (>95%) at 20 °C. These findings will consolidate the fundamental theories of room temperature catalytic reactions via constructing the SMSI interface engineering for wide environmental applications.
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APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING
·
2021
·Vol. 127
·期 12
·1-8
·
IF 2.584
Huang Yong,Li Pengcheng,Xu Liqun,Yu Yajie,Chen Wanping
Two kinds of WO 3 powders with average size of 100 nm and 5 μm have been used to prepare Pt–WO 3 porous composite ceramics, whose WO 3 grains are around 1 and 5 μm, respectively. The ceramics with 1 μm WO 3 grains show a sensitivity of 755 to 0.08% H 2 – 20% O 2 – N 2 in air of 30% relative humidity (RH) at room temperature, but show no response to this concentration of hydrogen in air of 50% RH due to the depression effect of water, which indicate a relatively low humidity tolerance for the ceramics. In contrast, the ceramics with 5 μm WO 3 grains show sensitivities of 1200 and 80 to 0.08% H 2 – 20% O 2 – N 2 at room temperature in air of 30% and 50% RH, respectively, and a sensitivity of 8 to 0.02% H 2 – 20% O 2 – N 2 in air of 70% RH, which represent an ultrahigh humidity tolerance. These results clearly demonstrate that the microstructure of room-temperature hydrogen sensitive metal oxide (MOX) materials exerts a decisive influence on their humidity tolerance. Much attention should be paid to MOX materials with large and even ultra-large MOX grains when room-temperature MOX gas sensors with high humidity tolerance are being developed.
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高影响因子
Journal of Energy Chemistry
·
2021
·
IF 9.676
Yihan Feng,Zichuang Li,Shanlin Li,Minghui Yang,Ruguang Ma,Jiacheng Wang
Integrating active Pt clusters into transition-metal oxides with water-dissociation ability is effective to prepare a bifunctional electrocatalyst for water splitting in alkaline. However, the additional utilization of a reductant and/or the operation at the elevating temperature causes the over-growth and agglomeration of Pt clusters, thus losing the high catalytic performance. Herein, we report that V dopant not only favors self-reducing Pt clusters on NiFe layered double hydroxide (LDH) (Pt/NiFeV) at room temperature, but also regulates interfacial charge redistribution to enhance the water-splitting performance. Experimental and theoretical studies reveal that V dopant into NiFe LDH triggers more electrons to transfer to adjacent Fe atoms, thus leading to a higher reducing ability compared to that without V-doping. When used as water-splitting electrocatalyst, V doping promotes electron loss of Pt clusters in Pt/NiFeV, optimizing the free energy of hydrogen adsorption and proton recombination kinetics at the cathode. Meanwhile, it also moves the d-band center of Ni away from the Fermi level to optimize the adsorption of *OH intermediates and facilitate the desorption of oxygen molecules at the anode. Thereby, Pt/NiFeV exhibits much higher bifunctional performance than V-free Pt/NiFe LDH toward both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). This work can spark inspiration of designing other bifunctional electrocatalysts for energy conversion and storage.
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CATALYSIS COMMUNICATIONS
·
2016
·
IF 3.389
Xingrui Fu,Yue Liu,Weiyuan Yao,Zhongbiao Wu
The catalytic performances of Pt-Pd/MCM-41 bimetallic catalysts prepared by one-step synthesis method were investigated for total toluene oxidation in this paper. The experimental results demonstrated that Pt-Pd/MCM-41 was of superior catalytic activity comparing to the monometallic Pt/MCM-41 or Pd/MCM-41 catalysts with the same metallic content, yielding an almost 100% conversion at 180 °C. The following characterization results indicated that the bimetallic catalyst possessed a higher surface Pt(0) content and smaller doped metal size owing to the synergistic effect of the two noble metals, resulting in the improvement of oxygen adsorption capacity and the reducibility.
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高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Wanzhen Zhu,Yu Meng,Chaoxin Yang,Jun Zhao,Hongliang Wang,Wei Hu,Guangqiang Lv,Yingxiong Wang,Tiansheng Deng,Xianglin Hou
As the frontier in heterogeneous catalyst, a monomer and positively charged active sites in the single-atom catalyst (SAC), anchored by high electronegative N, O, S, P, etc., atoms, may not be active for the multispecies (O2, substrates, intermediates, solvent etc.) involved liquid-phase aerobic oxidation. Here, with catalytic, aerobic oxidation of 5-hydroxymethylfurfural as an example, Pt SAC (Pt1-N4) was synthesized and tested first. With commercial Pt/C (Pt loading of 5 wt %) as a benchmark, 2,5-furandicarboxylic acid (FDCA) yield of 97.6% was obtained. Pt SAC (0.56 wt %) gave a much lower FDCA yield (28.8%). By changing the coordination atoms from highly electronegative N to low electronegative Co atoms, the prepared Pt single-atom alloy (SAA, Pt1-Co3) catalyst with ultralow Pt loading (0.06 wt %) gave a much high FDCA yield (99.6%). Density functional theory (DFT) calculations indicated that positively charged Pt sites (+0.712e) in Pt1-N4 almost lost the capability for oxygen adsorption and activation, as well as the adsorption for the key intermediate. In Pt1-Co3 SAA, the central negatively charged Pt atom (−0.446e) facilitated the adsorption of the key intermediate; meanwhile, the nearby Co atoms around the Pt atom constituted the O2-preferred adsorption/activation sites. This work shows the difference between the SAC with NPs and the SAA during liquid-phase oxidation of HMF and gives a useful guide in the future single-atom catalyst design in other related reactions.
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高影响因子
ACS Applied Energy Materials
·
2020
·
IF 4.473
Liting Cui,Zhengjian Li,Haining Wang,Lirui Cui,Jin Zhang,Shanfu Lu,Yan Xiang
It is of great significance to reduce the amount of platinum for the oxygen reduction reaction (ORR) in polymer electrolyte membrane fuel cells. In this work, a copper single atom coordinated by nitrogen doped carbon nanotubes is employed as a support for the deposition of platinum nanoparticles (Pt/Cu-SAC), according to the prediction of the density functional theory calculation, which reveals the ORR activity of Pt/Cu-SAC should be improved in comparison to that of Pt/C due to the weaker adsorption of oxygen. The prepared Pt/Cu-SAC exhibits more promising ORR activity than the commercial Pt/C due to the synergetic effect of Cu-SAC on the Pt particles. Furthermore, the fuel cell based on Pt/Cu-SAC with a cathode Pt loading of 0.025 mg cm–2 exhibits a peak power density of 526 mW cm–2, which is quite similar to that obtained with the commercial Pt/C with a cathode Pt loading of 0.1 mg cm–2. The Pt/Cu-SAC paves the way to design low-Pt cathode catalysts for the polymer electrolyte membrane fuel cells.
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高影响因子
Materials Today Nano
·
2021
·
IF 8.109
B. Yi,H. Zhao,L. Cao,X. Si,Y. Jiang,P. Cheng,Y. Zuo,Y. Zhang,L. Su,Y. Wang,C.-K. Tsung,L.-Y. Chou,J. Xie
Mixed-metal metal-organic frameworks (MM-MOFs) contain more than one type of metal node, which can improve or even introduce new features compared with the single metal frameworks. Traditionally, most of the MM-MOFs are synthesized by solution method which requires all the metal ions to form stable coordination with the ligand in a single framework and therefore limits the choice of the metal ions. In this work, Pt-doped Zn-MOF-74 (PtZn-MOF-74) has been prepared through a mechanochemical conversion approach from Pt-doped ZnO (Pt–ZnO) directly. The absence of a large quantity of solvent limits the solvation and diffusion of growth species during the mechanochemical conversion and therefore prevented the agglomeration of Pt dopants in PtZn-MOF-74. CO oxidation was used to evaluate the catalytic performance of the prepared MM-MOFs. Compared with inert Zn-MOF-74, PtZn-MOF-74 with unsaturated coordinated Pt at elevated temperature can act as the active sites to catalyze CO oxidation reaction. This study provides a novel design strategy for the synthesis of MM-MOFs with extended functionalities.
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高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2017
·Vol. 52
·期 18
·10738-10750
·
IF 2.599
Guo Leilei,Mao Long,Huang Kaixun,Liu Hongmei
In this paper, platinum (Pt)–selenium (Se) nanostructures and Pt nanoparticles were synthesized by a facile one-step chemical reduction route and their catalytic performance was evaluated as oxidase mimic. The results of structure characterization revealed that Pt – Se nanostructures consist of Pt and Se atoms (the Pt/Se atomic molar ratio is approximately 7:3), while Pt nanoparticles consist of pure element Pt. The oxidase-like activity of Pt – Se nanostructures and Pt nanoparticles was evaluated with 3,3′,5,5′-tetramethylbenzidine (TMB) as substrate. The results indicated that Pt – Se nanostructures had a lower Michaelis constant ( K
m ) and higher catalytic constant ( K
cat ) for TMB oxidation than that of Pt nanoparticles,which mean the binary Pt – Se hybrid nanostructures had stronger binding affinity with TMB and higher catalytic activity in comparison with monometallic Pt nanoparticles. The enhanced oxidase-like activity of Pt – Se nanostructures may be due to element Se doped in binary Pt – Se hybrid nanostructures, which can accelerate electron transport and provide excellent chemical stability against catalytic performance degradation during the TMB oxidation reaction. Mercury (II) ions (Hg 2+ ) could inhibit the oxidase mimetic activity of Pt – Se nanostructures and resulted in a color change of the reaction system. Based on this mechanism, a facile colorimetric assay for Hg 2+ was developed with a detection limit as low as 70 nm and a linear range of 0–2.5 μM.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2022
·
IF 12.92
Qing Yu,Shiyi Wang,Mengru Wang,Xiaoling Mou,Ronghe Lin,Yunjie Ding
Acetylene coupling with ethylene dichloride, which uses both coal and oil resources, is attractive for sustainable PVC manufacturing. Herein, highly active and stable carbon nitride-based catalysts were developed by a novel pre-oxidation-pyrolysis process, affording unprecedented dehydrochlorination activity with good durability. The best-performing system was further modified with different precious metals (Au, Pt, and Ru) to promote the hydrochlorination chemistry between the in-situ formed hydrogen chloride and acetylene co-feed. The presence of metal centers intensifies the hydrochlorination activity but weakens the dehydrochlorination ability due to competitive adsorption between the two reactants at the metal sites. Superior coupling performance was achieved over C 3 N 4 /AC and single-atom Au/C 3 N 4 /AC catalysts in cascade reactors. Our results strongly suggest that dehydrochlorination is an essential step in the coupling reaction, and the activation of acetylene and ethylene dichloride molecules requires different active sites that should be engineered in future work.
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高影响因子
BIOSENSORS & BIOELECTRONICS
·
2012
·
IF 5.602
Xiangheng Niu,Chen Chen,Hongli Zhao,Yan Chai,Minbo Lan
Novel snowflake-like Pt–Pd bimetallic nanoclusters (Pt–PdBNC) were synthesized on a screen-printed gold nanofilm electrode (SPGFE) substrate by electrochemically reducing precursors with a new constant potential/multi-potential step deposition strategy. The electrocatalytic behavior of the modified electrode (SPGFE/Pt–PdBNC) towards H 2 O 2 was investigated. The results indicate that the as-prepared Pt–PdBNC significantly enhances the electrochemical reduction of H 2 O 2 in neutral media, exhibiting preferable electrocatalytic performance compared to Pt and Pd monometallic nanoclusters . Under optimum conditions, SPGFE/Pt–PdBNC offers linear responses for H 2 O 2 in the concentration range from 0.005 to 6 mM with an ultrahigh sensitivity of 804 mA M −1 cm −2 and excellent selectivity. Furthermore, glucose oxidase was immobilized on the Pt–PdBNC structure, and the fabricated biosensor presents favorable properties for glucose sensing.
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高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2019
·Vol. 31
·期 1
·677-683
·
IF 2.195
Wang Jing,Shen Bowen,Zhu Kongjun,Qiu Jinhao
With the ever increasing requirements for the structural health monitoring systems, the deposition of the piezoelectric films on the metallic or structural materials has turned out to be an important issue. Pb(Mg, Nb)O 3 -PbTiO 3 films with different buffer layers, i.e., in situ NiO, pre-fabricated NiO and LaNiO 3 , were successfully deposited on the Ni foil via the chemical solution deposition. The crystal structures and electric performances showed evident dependence on the buffer layer. Pre-deposited NiO and LaNiO 3 efficiently prevented the diffusion and complex reactions occurring at the interface, offered abundant nucleation sites, and thus helped the formation of pure high-qualified perovskite PMN-PT films at higher annealing temperatures.
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