ACS Sustainable Chemistry & Engineering
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2023
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IF 8.4
Xilong Wang,Qinghua Zhang,Hechun Jiang,Yadong Li,Hongwei Zhu,Lirong Zheng,Lin Gu,Han-Pu Liang
Pt-based intermetallic alloys with high activity and stability are promising for accelerating the cathodic oxygen reduction reaction (ORR) and large-scale application of proton exchange membrane fuel cells. So far, facile synthesis of Pt-based alloys in less time is desirable but still challenging. Herein, based on the traditional wet impregnation method, facile in situ reduction of H2PtCl6 and alloying with a hybrid nanostructure mainly doped with Fe single atoms as well as small amounts of Fe-based nanoparticles and oxides were developed to fabricate highly dispersed PtFe nanoparticles loaded on a mesoporous Fe–N–C support. Alloying of Pt derived from H2PtCl6 with various iron-based species existing in forms of single-atom, metallic, and oxide states was confirmed by systematic characterization, and the Fe content in the support is important for PtFe alloy formation, and the corresponding electrochemical performance promotion has been identified. The as-synthesized best-performance PtFe/Meso-PDA-5 catalyst delivered a high potential of 0.925 V at a current density of 3 mA cm–2 and achieved a high mass activity of 497.5 mA mgPt–1 at 0.9 V for the ORR in 0.1 M HClO4. More importantly, only 17.9% mass activity loss was observed after 10k potential cycles of the accelerated deterioration test. The present work provides a strategy for facile synthesis of Pt-based alloy nanomaterials for ORR catalysis and highlights the importance of supports in alloy formation.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Manting Zhang,Tingting Zhou,Danil Bukhvalov,Fengyan Han,Caiqin Wang,Xiaofei Yang
Tri-functional PtCo/NC nanocatalysts were assembled via in-situ integration with ultralow Pt loading supported on ZIF-67 derived porous carbon material, and used as electrocatalysts for oxygen reduction reaction (ORR), ethanol oxidation reaction (EOR), hydrogen evolution reaction (HER). Detailedly, PtCo-3/NC with ultralow Pt loading (1 wt%) exhibits the halfwave potential of 0.877 V for ORR in acidic media and considerable current density for both ORR and EOR at 0.85 V, and low overpotential (η 10 =10 mV) for HER. The as-assembled zinc-air batteries (ZABs) based on PtCo/NC have higher power density than Pt/C based ZABs. DFT calculation reveals the strong metal-support interactions (MSI) in PtCo/NC, which leads to the change of electronic state, redistribution of charge density and optimization of free energy , allowing it to present greater performances than Pt/C. This work highlights the possibility of using it as highly effective electrode catalysts with ultralow Pt loading in fuel cells and metal-air battery.
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Journal of Energy Chemistry
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2023
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IF 13.1
Qiqi Mao,Wenxin Wang,Kai Deng,Hongjie Yu,Ziqiang Wang,You Xu,Xiaonian Li,Liang Wang,Hongjing Wang
Utilizing the hydrazine-assisted water electrolysis for energy-efficient hydrogen production shows a promising application, which relies on the development and design of efficient bifunctional electrocatalysts . Herein, we reported a low-content Pt-doped Rh metallene (Pt-Rhene) for hydrazine-assisted water electrolysis towards energy-saving hydrogen (H 2 ) production, where the ultrathin metallene is constructed to provide enough favorable active sites for catalysis and improve atom utilization. Additionally, the synergistic effect between Rh and Pt can optimize the electronic structure of Rh for improving the intrinsic activity. Therefore, the required overpotential of Pt-Rhene is only 37 mV to reach a current density of −10 mA cm −2 in the hydrogen evolution reaction (HER), and the Pt-Rhene exhibits a required overpotential of only 11 mV to reach a current density of 10 mA cm −2 in the hydrazine oxidation reaction (HzOR). With the constructed HER-HzOR two-electrode system, the Pt-Rhene electrodes exhibit an extremely low voltage (0.06/0.19/0.28 V) to achieve current densities of 10/50/100 mA cm −2 for energy-saving H 2 production, which greatly reduces the electrolysis energy consumption. Moreover, DFT calculations further demonstrate that the introduction of Pt modulates the electronic structure of Rh and optimizes the d -band center, thus enhancing the adsorption and desorption of reactant/intermediates in the electrocatalytic reaction.
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International Journal of Electrochemical Science
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2023
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IF 1.5
Shuxiao Chen,Hongda Du,Yinping Wei,Lingyi Peng,Yadong Li,Lin Gan,Feiyu Kang
We report the fabrication of electrospun antimony-doped tin oxides (ATO) nanofibers (NFs) with controlled cross-sectional architectures ranging from solid dense NFs via fiber-in-tube NFs to completely hollow tube-like NFs at otherwise constant conditions. These ATO NFs were further applied as catalyst supports on which Pt nanoparticles were electrodeposited. Our results show that the Pt nanoparticles deposited on the hollow ATO NFs exhibited a higher catalytic activity on oxygen reduction reaction compared to those supported on solid ATO NFs and conventional ATO powders. Transmission electron microscopy revealed that the Pt nanoparticles deposited on the hollow ATO NFs were spontaneously confined into the hollow channels of the NFs, which likely induced a nano-confinement effect and hence higher catalytic activity. Our results provide important insight into rational control of the mesostructures of metal oxides supported fuel cell catalysts for enhance catalytic properties.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Siyuan Hu,Mingzhen Huang,Jingru Li,Jinxin He,Kaiji Xu,Xiaoping Rao,Dongren Cai,Guowu Zhan
Herein, atomic layer deposition (ALD)-Al 2 O 3 films were applied as a medium to modulate the electronic states of the supported Pt. Based on the sacrificial template of ZIF-67, the ternary Co 3 O 4 /Pt/Al 2 O 3 catalyst exhibited better performance in catalytic CO oxidation than the binary Co 3 O 4 /Pt catalyst. Both experimental and calculation results indicate the existence of charge transport between the Pt and the ALD-Al 2 O 3 films, leading to electron-rich Pt, enhanced O 2 affinity, and reduced activation energy. Interestingly, the oxidation resistance of Pt nanoparticles was visualized when annealing Co 3 O 4 /Pt/Al 2 O 3 catalyst at high temperatures. Mechanism studies indicate the typical LH mechanism occurred in CO oxidation , showing that the co-adsorbed CO and O 2 could be converted to carbonate-type *OCOO intermediates via low energy barriers. At low temperatures, CO 2 was mainly produced by the lattice oxygen-mediated M-vK mechanism based on isotope labeling experiments. Our findings provide an alternative way to regulate the electronic states of noble metals by the ALD technique.
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FUEL
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2023
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IF 7.4
Fukun Bi,Shuting Ma,Bin Gao,Yang Yang,Lexun Wang,Fuhao Fei,Jingcheng Xu,Yuandong Huang,Minghong Wu,Xiaodong Zhang
Herein, Pd and Pt-catalysts loaded on non-oxide support (g-C 3 N 4 ) were prepared and compared for CO and toluene co-oxidation, and Pt/C 3 N 4 presented excellent catalytic performance. A series of characterizations including TEM, H 2 -TPR, O 2 -TPR and XPS etc., indicated that Pt/C 3 N 4 exhibited the smaller Pt NPs, better low temperature reduction ability, more active oxygen species and positive charged Pt species, which could account for its better catalytic performance. Additionally, DFT calculations further confirmed that the lower activation barrier of O 2 and the higher adsorption for CO and toluene triggered the efficient CO and toluene degradation over Pt/C 3 N 4 . Interestingly, the introduction of H 2 O (10.0 vol%) suppressed the catalytic performance of Pd/C 3 N 4 , while expedited CO and toluene oxidation over Pt/C 3 N 4 , which was revealed by DFT calculations. Furthermore, the difference in degradation intermediates, corresponding distributions and toxicity generated during toluene oxidation under different conditions over Pd/C 3 N 4 and Pt/C 3 N 4 were exposed. Compared with Pd/C 3 N 4 , less variety, toxicity and content of intermediates produced over Pt/C 3 N 4 . This work would inspire many rational designs of supported noble metal catalysts for environmentally friendly catalysis.
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ELECTROCHIMICA ACTA
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2023
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IF 6.6
Jiarun Cheng,Chaojie Lyu,Gang Dong,Yongqiang Liu,Yue Hu,Bin Han,Dongsheng Geng,Dongjie Zhao
Highly efficient and stable Pt-based electrocatalysts have broad application prospects in fuel cells, among which, Pt loading accompanied with particle size, interparticle distance (ipd), and interaction with support are identified as key contributors for high activity and selectivity. Herein, we have developed the nitrogen-doped graphite-like carbon sheets supporting low-Pt loading (Pt@N-GC) with uniform size and controllable ipd, and disentangled the main effect of ipd on oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR) activity. The optimal 5.0 wt% low-Pt loading results in more abundant Pt sites and lower ipd, which leads to the higher surface reactivity by proximity effect , and 2e − pathway can be hindered by strongly resorbing and reducing H 2 O 2 to promote 4e − pathway towards ORR . Simultaneously, the 5.0 wt% Pt@N-GC can effectively improve the MOR activity, enhance the adsorption of -OH group under the appropriate ipd, so as to promote the instantaneous oxidation of CO and enhance the tolerance, and accelerate the oxidative dehydrogenation of methanol. Benefiting by the synergistic effect of Pt nanoparticles and N-GC support, all Pt@N-GCs exhibit bifunctional electrocatalytic activity and durability. We believe the gained trade-off of the loading and proximity effect of Pt, and its influence on catalytic activity and selectivity contributes to design more promising low-Pt loading bifunctional catalysts for fuel cell.
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INTERNATIONAL JOURNAL OF ENERGY RESEARCH
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2019
·Vol. 43
·期 6
·2075-2085
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IF 3.343
Rong Dai,Ziliang Zheng,Chenshuai Lian,Xing Li,Xu Wu,Xia An,Xianmei Xie
Summary A novel Pt-based Beta encapsulated CeO 2 yolk-shell catalyst was successfully synthesized via a RF layer in the synthetic process. The CeO 2 @Pt-Beta catalyst showed high catalytic activity and stability toward the LT-ESR with respect to the reference Pt-Beta, CeO 2 -Pt-Beta, which benefited from the special yolk-shell structure and the synergistic effect between the CeO 2 movable core and Pt metal. The confinement effect of the yolk-shell architecture contributed to the high dispersion of Pt nanoparticles as well as to the accumulation of reactant molecules in the enclosed void space, which ensured the reactants reacted with CeO 2 and Pt to achieve a complete reaction.
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APPLIED CATALYSIS A-GENERAL
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2019
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IF 4.63
Xin Zhang,Jianfeng Zhang,Huiyang Cao,Yahui Li
Although direct methanol fuel cells are promising as “green” power generators for portable electronics, their further development has been largely hampered by the low-efficiency of the commercial anode catalysts. In this study, (Ti 3 C 2 T x ) y -(MWCNTs) 1- y (0 ≤ y ≤1) supported Pt nanoparticle electrocatalysts were fabricated by a facile and scalable solvothermal strategy, after which two-dimensional(2D) Ti 3 C 2 T x nanosheets were found to be intercalated and connected by conductive one-dimensional(1D) MWCNTs. Used for methanol oxidation reaction, the Pt/(Ti 3 C 2 T x ) 0.5 -(MWCNTs) 0.5 catalyst exhibited the maximum electrochemical active surface area (ECSA, 154 m 2 /g) and excellent electrochemical activity (812.9 mA/mg), higher than not only Pt/Ti 3 C 2 T x and Pt/MWCNTs of this study, but also many other related catalysts reported in literature. In addition, the CO-poisoning behavior was also alleviated using Pt/(Ti 3 C 2 T x ) 0.5 -(MWCNTs) 0.5 instead of Pt/Ti 3 C 2 T x and Pt/MWCNTs. Such a superior performance can be attributed to the well dispersion of Pt nanoparticles (∼3.8 nm), enhanced layer distance of Ti 3 C 2 T x to capture more Pt nanoparticles, and conductive action of MWCNTs to connect Ti 3 C 2 T x . This study opens a new perspective for developing high performance supercapacitors using Pt catalysts supported by 1D-intercalated 2D materials.
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
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2019
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IF 4.029
Xudong Qi,Yan Zhao,Enwei Sun,Juan Du,Kai Li,Ye Sun,Bin Yang,Rui Zhang,Wenwu Cao
The photoluminescence , dielectric relaxation, ferroelectric hysteresis, and field-induced strain properties of Pr 3+ -doped 0.24Pb(In 1/2 Nb 1/2 )O 3 -0.42Pb(Mg 1/3 Nb 2/3 )O 3 -0.34PbTiO 3 (PIN-PMN-PT:Pr 3+ ) multifunctional ceramics have been investigated. It was found that Pr 3+ doping enhanced the dielectric diffuseness and relaxation behavior of PIN-PMN-PT ceramics. Slim P - E loops and S - E curves appear in PIN-PMN-PT:Pr 3+ ceramics when the Pr 3+ doping concentration reaches 1.4 mol%. Local domain configurations associated with phase transitions were investigated by piezoresponse force microscopy (PFM). Large electrostrictive coefficient Q 33 (˜0.03 m 4 /C 2 ) and high energy-storage efficiency η (92%) were obtained in 2 mol% Pr 3+ -doped PIN-PMN-PT ceramic in the ergodic relaxor (ER) phase at room temperature. The giant electrostrictive effect and excellent energy-storage performance are related to the field-induced dynamic behavior of polar nanoregions (PNRs). The results show that the PIN-PMN-PT:Pr 3+ system is an excellent multifunctional material for making electromechanical and energy storage devices.
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Journal of Pharmaceutical Analysis
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2019
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IF 4.44
Satar Tursynbolat,Yrysgul Bakytkarim,Jianzhi Huang,Lishi Wang
The simultaneous electrochemical determination of myricetin and rutin remains a challenge due to their indistinguishable potentials. To solve this problem, we constructed a ternary platinum nanoparticle, reduced graphene oxide, multi-walled carbon nanotubes (Pt@r-GO@MWCNTs) nanocomposite via a facile one-pot synthetic method. Under the optimized conditions, the ternary Pt@r-GO@MWCNTs nanocomposite exhibited good electrocatalytic activity toward myricetin and rutin via solid phase extraction and excellent performance for the simultaneous determination of myricetin and rutin. The oxidation peak current of myricetin was proportional to its concentrations in the range of 0.05–50 μM with a detection limit of 0.01 μM (S/N = 3). The linear range for rutin was 0.05–50 μM with a detection limit of 0.005 μM (S/N = 3). The ternary nanocomposite sensor also exhibited good reproducibility and stability, and was successfully used for the simultaneous determination of myricetin and rutin in real orange juice samples with recoveries ranging between 100.57% and 108.46%.
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PubMed
高影响因子
ChemCatChem
·
2019
·Vol. 11
·期 9
·2362-2369
·
IF 4.495
Xue Zhao,Yunfan Fu,Chen Yao,Shuran Xu,Yu Shen,Qiong Ding,Wenjing Liu,Haibo Zhang,Xiaohai Zhou
Graphical A closo case : In situ preparation of ultrafine Pd and Pt nanoparticles on dodecahydro-closo-dodecaborate organic polymers for high efficiency catalytic hydrolytic dehydrogenation of ammonia borane. Using in situ reduction strategy by combining organic frameworks and ultrafine Pd and Pt nanoparticles (Pd−NPs and Pt−NPs) to synthesize composites with tunable morphology and high dispersion has attracted extensive attentions in fabrication of composite nanomaterials. Herein, on the new kind of substrate, BOPs@Pd and BOPs@Pt nano materials have been successfully fabricated via in situ reduction of Na 2 PdCl 4 and H 2 PtCl 6 triggered by reducibility of organic boron polymers (BOPs). The final products are obtained by loading Pd−NPs and Pt−NPs with ultra-small size and high dispersion without any tedious chemical modification or additional additives. These materials show high catalytic activity and recyclability in the hydrolysis dehydrogenation of ammonia borane (AB).
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