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Chemistry-An Asian Journal · 2020 ·Vol. 15 ·期 20 ·3356-3364 · IF 4.056

Kinetically Manipulating the Nucleus Attachment to Create Atypical Defective Rh−Pt Alloyed Nanostructures as Active Electrocatalysts

Kai Liu,Zixi Lyu,Xuejiao Chen,Xinyan Liao,Guanhong Chen,Xin Lin,Wei Wang,Shuifen Xie

Graphical A selective synthesis of atypical Rh−Pt alloyed nanocrystals with different morphologies and defective structures has been achieved through kinetically manipulating the nucleation and nucleus attachment. The defective Rh 47 Pt 53 wavy nanowires endowed with abundant grain boundaries and twin boundaries present a superior electrocatalytic performance for the ethanol oxidation reaction. Defective metal nanostructures have attracted great attention due to the striking catalytic behavior of the defect sites. Atypical metal nanocrystals generated from attached nuclei can accommodate abundant grain boundaries (GBs) and twin boundaries (TBs). However, the understanding of their growth-mechanism and precisely synthetic control over such defective nanocrystals are still scarce. Herein, using the Rh−Pt nanoalloy as a model system, we systematically demonstrate that a prudent control of the reaction kinetics can manipulate the metal nucleation and nucleus attachment to create atypical nanocrystals, including small isolated nanoparticles (NPs), defect-rich wavy nanowires (WNWs), and {100} facet-bounded spliced nanocubes (SNCs). In the ethanol oxidation electrocatalysis, the Rh 47 Pt 53 WNWs featured with abundant TBs and GBs show the greatest mass activity (0.655 A ⋅ mg −1 Pt , 2.9 times to the commercial Pt/C) and durability. Our work captures the core of reaction kinetics on regulating the nucleus attachment and enables the rational control over the nanocrystal morphology and defect.

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PROCEEDINGS OF THE COMBUSTION INSTITUTE · 2020 · IF 5.627

Flame spray pyrolysis made Pt/TiO2 photocatalysts with ultralow platinum loading and high hydrogen production activity

Fuchang Gao,Zuwei Xu,Haibo Zhao

In this paper, flame spray pyrolysis (FSP) is used to synthesize Pt/TiO 2 catalysts with surface-supported isolated Pt atoms through elaborate precursor/solvent formulation and flame temperature history control. It is a pivotal factor to this FSP process that there is a major distinction on saturated vapor pressure between two components (Pt species and Ti species), and thereby they exist as gas phase and particle phase at a certain temperature range, respectively. When the flame is quenched to ambient temperature with cold sheath gas , Pt species of gaseous PtO 2 (being in the vapor phase above 723 K) condense into deposition state on the surface of TiO 2 nanoparticles . Combined with X-ray photoelectron spectroscopy (XPS) analysis and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) detection, we identify that Pt atoms are dispersed and anchored on the catalyst surface . Single-atom Pt dispersed Pt/TiO 2 catalysts can be well achieved by controlling the loading at a very low level, which offers an effective way to maximize the atom economy for surface catalysis of scarce noble metals. In this work, considering that Pt as the best co-catalyst of hydrogen evolution, the FSP-made Pt/TiO 2 catalysts are tested in a photocatalysis water splitting system aiming to a simple and attractive means of renewable hydrogen production . The highest activity presents in 0.1Pt/TiO 2 with 0.1% molar ratio of Pt to Ti, reaching 108.5 times of the benchmark sample from commercial flame-made TiO 2 (P25). The high activity is attributed to the fact that the isolated Pt atom serves as the main active site for photocatalysis hydrogen evolution. Therefore, the performance and cost efficiency of catalysts are greatly improved by the FSP, mainly ascribed to engineering atomically dispersing Pt on the support surface.

CAS / MDL: 15170-57-7
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RARE METALS · 2021 ·Vol. 41 ·期 2 ·630-638 · IF 4.003

Au@Ag@Pt core–shell nanorods regulating Ag release behavior endow titanium antibacterial activity and biocompatibility

Qiu Jia-Jun,Yang Ting-Ting,Li Yi-Fan,Qian Wen-Hao,Liu Xuan-Yong

Although titanium and its alloys are extensively used in orthopedics and dentistry fields, implant failures still happen because of implant-associated infections. Herein, Au@Ag@Pt core–shell nanorods with noble metal combination were fabricated and assembled on medical titanium surface and the antibacterial activity and biocompatibility were investigated. The results showed that antibacterial rates of Ti–Au@Ag@Pt against S. epidermidis and P. aeruginosa were 89.7% and 92.7%, respectively. Besides, Ti–Au@Ag@Pt showed no obvious cell toxicity with MC3T3-E1 cells grew well on the sample surface. It was discovered that the Pt shell layer on Ti–Au@Ag@Pt slowed down the Ag ion release rate which endowed medical titanium surface with both antibacterial activity and good biocompatibility. Graphical abstract

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MICROCHIMICA ACTA · 2020 ·Vol. 187 ·期 4 ·1-7 · IF 6.232

Colorimetric determination of Pb2+ ions based on surface leaching of Au@Pt nanoparticles as peroxidase mimic

Xie Zheng-Jun,Shi Mei-Rong,Wang Li-Ying,Peng Chi-Fang,Wei Xin-Lin

We report the first use of metallic nanozyme as colorimetric probe for Pb 2+ determination. The method is based on the surface leaching of Au@PtNP nanozyme by Pb 2+ -S 2 O 3 2− ions, accompanied by a decreased catalytic activity of the metallic nanozyme. To construct this colorimetric determination, the Pt deposition onto the AuNPs was carefully investigated and other experimental factors including kind of substrate and buffer were optimized. With increasing Pb 2+ concentration, the catalytic activity of the Au@PtNPs decreased gradually. As a result, the blue color at 650 nm from the oxidation of 3,3′,5,5′-tetramethylbenzidine by H 2 O 2 faded gradually. A determination limit of 3.0 nM Pb 2+ with a linear range from 20 to 800 nM was obtained. The assay demonstrated negligible response to common metal ions even at elevated concentrations. This colorimetric method was applied to the determination of Pb 2+ ions spiked in lake water samples, and good recoveries (96.8–105.2%) were obtained. The above results indicate the potential application of metallic nanozymes in developing robust colorimetric assays. Schematic representation of the surface leaching of Au@PtNP nanozyme by Pb 2+ -S 2 O 3 2− ions, accompanying the decreased catalytic activity of the metallic nanozyme

CAS / MDL: 7772-98-7 54827-17-7
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Low Pt-Content Ternary PtNiCu Nanoparticles with Hollow Interiors and Accessible Surfaces as Enhanced Multifunctional Electrocatalysts

Dengfeng Wu,Wei Zhang,Aijun Lin,Daojian Cheng

Developing highly active and durable electrocatalysts with low levels of Pt content toward some crucial reactions including oxygen reduction reaction, hydrogen evolution reaction, and methanol oxidation reaction in an acidic electrolyte environment are desirable but still an open challenge for clean and efficient energy conversion. Herein, we present a facile route to synthesize low Pt-content ternary PtNiCu nanostructures with hollow interior and accessible surfaces (H-PtNiCu-AAT NPs) as enhanced multifunctional electrocatalysts. The galvanic replacement reaction and atomic diffusion between in situ preformed CuNi nanocrystals and Pt species should be responsible for the formation of hollow PtNiCu NPs. Continuous activation by acid picking and annealing treatments were performed to leach out the excessive Cu and Ni on the surfaces and to enrich Pt-content on the surface. H-PtNiCu-AAT NPs exhibit excellent activity and durability toward HER, ORR, and MOR due to the rational integration of multiple structural advantages. Strikingly, the mass activity and specific activity of H-PtNiCu-AAT NPs (0.977 A mgPt–1 and 1.458 mA cm–2) is 7.1 and 6.9 times higher than that of commercial Pt/C (0.138 A mgPt–1 and 0.212 mA cm–2) toward ORR at 0.9 V (vs RHE), respectively. This present work provides an efficient strategy for the design of low Pt-content trimetallic electrocatalysts with excellent activity and durability.

CAS / MDL: 7791-20-0 112-90-3
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JOURNAL OF MATERIALS SCIENCE · 2020 ·Vol. 55 ·期 26 ·11829-11840 · IF 3.553

Metallic Pt and PtOx dual-cocatalyst-loaded WO3 for photocatalytic production of peroxydisulfate and hydrogen peroxide

Xie Wenwen,Huang Zeai,Wang Ruiqi,Wen Cheng,Zhou Ying

Photocatalytic production of green oxidation reagents as an economical and environmental-friendly process is a promising strategy to replace the traditional production processes. In the present study, a series of 1.0 wt% Pt/WO 3 photocatalysts with different surface chemical states of Pt were successfully fabricated. The different surface metallic Pt (Pt 0 ) and oxidized Pt (PtO x ) ratios on WO 3 showed significant effects on the photocatalytic activities for strong oxidants of peroxydisulfate ( \( {\text{S}}_{ 2} {\text{O}}_{8}^{2 - } \) ) and hydrogen peroxide (H 2 O 2 ) formations. It is proposed that surface Pt 0 and PtO x functioned as reduction site for O 2 reduction to H 2 O and oxidation site for H 2 O oxidation to H 2 O 2 , respectively, during the photocatalytic process. As a result, a higher surface composition of Pt 0 prepared using photodeposition (PD) method led to the formation of higher amount of \( {\text{S}}_{ 2} {\text{O}}_{8}^{2 - } \) . On the other hand, PtO x -loaded WO 3 using impregnation (IM) method showed significant formations of \( {\text{S}}_{ 2} {\text{O}}_{8}^{2 - } \) and H 2 O 2 simultaneously. This work provided a new idea for the design of noble metal Pt-supported WO 3 for efficiently photocatalytic generation of \( {\text{S}}_{ 2} {\text{O}}_{8}^{2 - } \) and H 2 O 2 .

CAS / MDL: 16941-12-1
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Synthesis of Intermetallic Pt-Based Catalysts by Lithium Naphthalenide-Driven Reduction for Selective Hydrogenation of Cinnamaldehyde

Xiao Chen,He Cao,Xiaozhen Chen,Yan Du,Ji Qi,Jingjie Luo,Marc Armbrüster,Changhai Liang

Intermetallic nanoparticles (NPs) with a well-defined atom binding environment and a long-range ordering structure can be used as ideal models to understand their physical and catalytic properties. In this work, several kinds of nanostructured and carbon nanotube (CNT)-supported Pt-based intermetallic compounds (IMCs) have been synthesized by one-step lithium naphthalenide-driven reduction at room temperature without the use of surfactants in light of the reduction potential of metals. In the chemoselective hydrogenation of cinnamaldehyde, the second metal in Pt-M IMCs significantly creates a suitable reaction environment through construction of a good geometric and electronic structure. The Pt3Sn/CNT catalyst presents highly efficient and good chemoselective hydrogenation of cinnamaldehyde to cinnamyl alcohol. This can be attributed to the fact that the incorporated Sn atoms effectively dilute large Pt ensembles and increase the electron density of Pt. The in situ-formed SnOx interfaces as Lewis acid sites facilitate the coordination of C═O bonds, enhancing the selectivity to cinnamyl alcohol. In addition, the SnOx interface as the joint between Pt3Sn IMCs NPs and CNTs significantly improves the stability of the catalyst in the reaction environment.

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CATALYSIS SURVEYS FROM ASIA · 2020 ·Vol. 24 ·期 2 ·104-114 · IF 2.194

Bimetallic Bifunctional Pt-NiP/Hβ as a Novel and Highly Efficient Catalyst for n-Hexane Isomerization

Yang Lijuan,Song Zhaoyang,Yu Yingmin,Zhu Lijun,Xia Daohong

A novel bimetallic bifunctional Pt–NiP/Hβ isomerization catalyst was successfully prepared by introducing a small amount of noble metal Pt into the NiP on the Hβ carrier. The catalyst demonstrated superior catalytic activity to Pt/Hβ and NiP/Hβ catalysts for n -hexane isomerization, due to the good surface property, the synergistic effect of the two metals, the suitable match between acid site and metal site, as well as good reduction stability. The effects of Pt loading and NiP addition amount on the surface property were studied comprehensively through a series of characterization, and the correlation among surface property with catalytic behavior was also analyzed. The results indicated that the Pt (0.1 mol%)–NiP (10 mol%)/Hβ catalyst had good structural characters, surface acid property and an uniform distribution of NiP and Pt active components on surface, which is helpful to obtain a highly efficient catalytic performance. Additionally, the influence of reduction/reaction conditions on the catalytic activity, as well as the catalyst tolerance to water and thiophene sulfur, was investigated furtherly.

CAS / MDL: 6303-21-5 102-69-2
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

In Situ Encapsulation of Pt Nanoparticles within Pure Silica TON Zeolites for Space-Confined Selective Hydrogenation

Junjie Tang,Peiwen Liu,Xiaoling Liu,Lei Chen,Haimeng Wen,Yu Zhou,Jun Wang

Straightforward encapsulation of Pt clusters (∼2 nm) into the pure silica TON-type zeolite (ZSM-22) was reached in a dry gel conversion route, where the ionic liquid template was removed via the hydrocracking-calcination-reduction approach. The obtained Pt@ZSM-22 series possessed high crystallinity, large surface area, and ultrafine Pt clusters inside the zeolite crystals. They exhibited remarkable activity in the semi-hydrogenation of phenylacetylene into styrene; the lead sample with 0.2 wt % Pt loading afforded a large turnover number up to 117,787. The preferential high affinity of the pure silica ZSM-22-encapsulated Pt clusters toward the substrate phenylacetylene rather than the hydrogenated product was derived from the unique space-confinement effect of zeolite microchannels, which is responsible for such excellent performance.

CAS / MDL: 16941-12-1 4420-74-0
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ACS Applied Nano Materials · 2020 · IF 0

Pt Nanoparticles Supported on N-Doped Porous Carbon Derived from Metal–Organic Frameworks for Oxygen Reduction

Chao Wang,Xiaodan Wang,Fengyu Lai,Zheng Liu,Ruohao Dong,Wen Li,Hongxia Sun,Baoyou Geng

Metal–organic framework (MOF)-derived materials have attracted increasing attention in the field of energy storage and conversion. Calcining MOFs to carbonized structures is a common route to obtain MOF-derived materials. However, the existing calcination conditions often cause the structural collapse and the specific surface area to be significantly reduced. In this work, we use argon–hydrogen mixed gas for calcination of MOFs to obtain a N-doped porous carbon material with excellent properties. Its BET specific surface area and pore volume up to 2476 m2 g–1 and 1.325 cm3 g–1, respectively, which are higher than those of the precursor ZIF-8 (1960 m2 g–1 and 0.687 cm3 g–1), perfectly inherited the rhombic dodecahedron morphology of the precursor. Hydrogen reduces the zinc in ZIF-8 at high temperature to evaporate, which avoids the carbothermal reduction reaction between the zinc component and the carbon framework of MOFs, protecting the framework of MOFs and leaving a lot of micropores, so that after the carbonization of MOFs it still has extremely high specific surface area and pore volume, even surpassing the MOFs precursors. We loaded Pt nanoparticles on the prepared porous carbon to catalyze the oxygen reduction reaction and showed an excellent half-wave potential of 0.883 V, which is 10 mV higher than that of the commercial Pt/C (Pt 20 wt %), while the Pt loading is only 8.66 wt %. The stability is also much better than Pt/C.

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JOURNAL OF POWER SOURCES · 2020 · IF 8.247

Electric field-assisted synthesis of Pt, carbon quantum dots-coloaded graphene hybrid for hydrogen evolution reaction

He Xiao,Jingjuan Zhang,Man Zhao,Jianchun Ma,Ya Li,Tianjun Hu,Zhanfeng Zheng,Jianfeng Jia,Haishun Wu

A simple method for preparation of Pt, CQDs-coloaded graphene composite for hydrogen evolution reaction (HER) is established by electrolysis-solvothermal process. Graphene is obtained by electrochemical exfoliation of graphite in cathode, while carbon quantum dots (CQDs) and Pt nanoparticles (NPs) are in-situ generated in the electrolyte simultaneously. CQDs are evolved from propylene carbonate solvent and Pt NPs are derived from reduction of Pt intermediate species generated from anodic dissolution of Pt counter electrode during electrolysis process. Then Pt NPs and CQDs are well dispersed on graphene at subsequent solvothermal process. Work voltage and electrolyte type as the key electrolysis conditions are applied to control the concentration of CQDs and Pt NPs, which decides electrochemically active surface area and HER activity of obtained catalysts. Significantly, the obtained superior catalyst with trace amount of Pt (0.145 wt%), shows markedly enhanced catalytic HER activity with mass activity of 37.5 A mg −1 at −50 mV in acidic solution, 68.2 times more active than Pt/C. This study provides a universal and promising methodology for synthesizing Pt, CQDs coloaded hybrid with the assistance of electric field as cost-effective catalysts for fuel cells.

CAS / MDL: 68-12-2 108-32-7
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2021 · IF 4.464

Electrochemical synthesis of Pt nanoparticles on ZrO2/MWCNTs hybrid with high electrocatalytic performance for methanol oxidation

Haoye Wang,Yun Yang,Yihan Ren,Duangui Chen,Jianhong Wei,Lu Wang,Aijuan Xie,Shiping Luo

Zirconia supported on multi-walled carbon nanotubes (ZrO 2 /MWCNTs) as carriers was synthesized with hydrothermal method, and then ternary Pt-ZrO 2 /MWCNTs hybrid was prepared by electrodeposition with aims to enhance electron and proton conductivity, specific surface as well as active site, and also oxidize the adsorbed CO on Pt surface and synergistically improve electrocatalytic activity and stability for the oxidation of methanol. The synthetic conditions of Pt-ZrO 2 /MWCNTs, such as mass ratio of ZrO 2 /MWCNTs, deposition cycle of Pt, were screened, respectively. The catalytic performance of Pt-ZrO 2 /MWCNTs hybrid for methanol oxidation was investigated by cyclic voltammetry, electrochemical impedance spectroscopy, and chronoamperogram test. The results showed that Pt-ZrO 2 /MWCNTs hybrid exhibited significantly lower charge transfer resistance and better toxicity resistance compared with the commercial Pt/C(20 wt%)-SA. Meanwhile, the ECSA (42.25 m 2 /g) of Pt-ZrO 2 /MWCNTs hybrid is higher than that of other related materials. Therefore, the as-prepared Pt-ZrO 2 /MWCNTs hybrid is a promising electro-catalyst for the application of direct methanol fuel cell.

CAS / MDL: 308068-56-6
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