ADVANCED FUNCTIONAL MATERIALS
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2022
·Vol. 32
·期 38
·2202675
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IF 19.924
Mingzhen Hu,Zengjian Cai,Xinhu Liang,Ganggang Li,Haiyan Tan,Shitu Yang,Hao Ren,Zhe Wang,Guodong Sun,Shoujie Liu,Zhengping Hao,Kebin Zhou
It is extremely challenging to controllably synthesize rare earth-containing nanoalloys due to the ultralow standard reduction potential of rare earth metals. Here, a surface-confined strategy to prepare ultrafine Pt-rare earth nanoalloys on a series of N-functionalized supports is reported. It proves that by surface N-metal coordination, the metal cations of precursors are atomically dispersed on support, which greatly favors uniform nucleation and growth of particles upon reduction. Moreover, the moderate metal transfer barrier from N ensures particle growth in a confined region to form ultrafine nanoalloys. Using this method, ultrafine Pt La, Pt Y, and Pt Dy nanoalloys are prepared on N-functionalized supports such as carbon, zeolite, and Al 2 O 3 . Notably, the Pt La nanoalloys on N-functionalized zeolite show superior activity and durability for propane oxidation. The strategy is expected to provide guidelines for preparing highly efficient rare earth-containing nanoalloys for catalysis applications.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Wang Zhe,Wang Chunpeng,Mao Shanjun,Lu Bing,Chen Yuzhuo,Zhang Xie,Chen Zhirong,Wang Yong
Decoupling the electronic and geometric effects has been a long cherished goal for heterogeneous catalysis due to their tangled relationship. Here, a novel orthogonal decomposition method is firstly proposed to settle this issue in p -chloronitrobenzene hydrogenation reaction on size- and shape-controlled Pt nanoparticles (NPs) carried on various supports. Results suggest Fermi levels of catalysts can be modulated by supports with varied work function ( W f ). And the selectivity on Pt NPs of similar size and shape is linearly related with the W f of support. Optimized Fermi levels of the catalysts with large W f weaken the ability of Pt NPs to fill valence electrons into the antibonding orbital of C–Cl bond, finally suppressing the hydrodehalogenation side reaction. Foremost, the geometric effect is firstly spun off through orthogonal relation based on series of linear relationships over various sizes of Pt NPs reflecting the electronic effect. Moreover, separable nested double coordinate system is established to quantitatively evaluate the two effects.
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RSC Advances
·
2022
·Vol. 12
·期 35
·22565-22573
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IF 4.036
Dashu Pan,Yubing Xue,Songtao Xiao,Yinggen Ouyang,Feng Zuo,Fuyan Lou,Xiang Li
Radioactive UO2 powder was prepared by hydrothermal method and a set of Pt–xUO2/C catalysts were synthesized by impregnation method for solving the problem of low activity and easy poisoning of anode Pt/C catalysts for a direct ethanol fuel cell. XRD, TEM, EDS, XPS and ICP-MS characterization showed the successful loading of Pt and UO2 onto the carbon carrier. Electrochemical workstation and single cell test results confirm that the catalytic performance of Pt–10% UO2/C is significantly better than Pt/C-eg. It is speculated that the synergistic effect of Pt and U enhances the catalytic activity and UO2 improves the resistance to CO poisoning by releasing O2 stored in the lattice space, while the α-particles released by 235U can also generate radiolysis product OH and promote the oxidative desorption of CO from the Pt surface.
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AICHE JOURNAL
·
2022
·Vol. 68
·期 12
·e17852
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IF 4.167
Yang Zhao,Xinyi Zhang,Jiarui Yang,Mingyu Gao,Pengfei Yang,Qian Wang,Dianqing Li,Junting Feng
In this work, a commercial P25 (TiO 2 ) with phase junctions between (101) and (110) faces supported Pt catalyst was prepared for glycerol selective oxidation, giving a decent 76.8% glyceric acid (GLYA) yield, and good stability. The kinetic experiments calculated apparent activation energy, turnover frequency (TOF), and reaction rates, demonstrating Pt/P25 could facilitate glyceraldehyde (GLYAD) formation and inhibit GLYA over-oxidation. Series of structural techniques confirmed the 101/110 junctions in P25 contributed electronic effect on Pt through metal-support interface, which improved the oxygen activation ability and optimized the GLYAD/GLYA adsorption modes. Furthermore, progressive scale-up reactions were tested and the mass transfer limitations under different conditions were thoroughly studied. The obtained mass transfer factors suggested the gas–liquid and liquid–solid mass transfer were severely limited. Finally, through optimizing the conditions, Pt/P25 catalyst achieved 75.8% GLYA yield at 300 ml-scale reaction, realizing equivalent magnification with the 5 ml-scale experiment.
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SENSORS AND ACTUATORS B-CHEMICAL
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2022
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IF 9.221
Zinan Zhi,Wanshuo Gao,Jiawei Yang,Chong Geng,Boxuan Yang,Chen Tian,Shurui Fan,Haoyi Li,Jinpo Li,Zhongqiu Hua
In the present work, an amperometric electrochemical hydrogen (H 2 ) sensor was fabricated by solid polymer electrolyte and screen-printed electrodes (SPE). The carbon electrode modified by Pt/C/Nafion film gave an enhanced sensitivity. The Pt/C/Nafion suspension could be directly added dropwise to the carbon electrodes for modification, which was simple and efficient. For hydrogen sensors, it was proved that hydrogen and Pt nanoparticles in aprotic electrolyte were the electrochemical behavior of single electron transfer in an anaerobic environment and the coupling electrochemical behavior with oxygen in an aerobic environment. A solid amperometric gas sensor was fabricated by a 3D printing package with a solid polymer electrolyte and porous ceramic subtracts printed with modified electrodes. It was indicated that the sensor device fabrication was quite simple; however, the sensitivity could be greatly improved.
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Crystals
·
2022
·Vol. 12
·期 6
·778
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IF 2.67
Shunhong Dong,Juan Wu,Lanlan Huang,Hong-En Wang
Narrowing the band gap and increasing the photodegradation efficiency of TiO2-based photocatalysts are very important for their wide application in environment-related fields such as photocatalytic degradation of toxic pollutants in wastewater. Herein, a three-dimensionally ordered macroporous Pt-loaded TiO2photocatalyst (3DOM Pt/TiO2) has been successfully synthesized using a facile colloidal crystal-template method. The resultant composite combines several morphological/structural advantages, including uniform 3D ordered macroporous skeletons, high crystallinity, large porosity and an internal electric field formed at Pt/TiO2interfaces. These unique features enable the 3DOM Pt/TiO2to possess a large surface for photocatalytic reactions and fast diffusion for mass transfer of reactants as well as efficient suppression of recombination for photogenerated electron-hole pairs in TiO2. Thus, the 3DOM Pt/TiO2exhibits significantly enhanced photocatalytic activity. Typically, 88% of RhB can be degraded over the 3DOM Pt/TiO2photocatalyst under visible light irradiation (λ ≥ 420 nm) within 100 min, much higher than that of the commercial TiO2nanoparticles (only 37%). The underlying mechanism for the enhanced photocatalytic activity of 3DOM Pt/TiO2has been further analyzed based on energy band theory and ascribed to the formation of Schottky-type Pt/TiO2junctions. The proposed method herein can provide new references for further improving the photocatalytic efficiency of other photocatalysts via rational structural/morphological engineering.Keywords:3D ordered macropores;TiO2;Pt loading;photocatalysis;Schottky junction
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Frontiers in Chemistry
·
2022
·
IF 5.545
Cao Xiaochang,Qiu Zhongming,Chen Jianjun,Ai Tianyu
Direct ethanol fuel cells (DEFCs) have attracted more and more attention because of their unique advantages such as low cost and low toxicity. However, sluggish C-C bond cleavage during the ethanol electrooxidation reaction (EOR) in acidic media results in a lower energy yield and gravely hinders the commercialization of DEFCs. Therefore, it is very necessary to develop an anode catalyst with high performance, high stability and low cost to solve this problem. In this paper, Pt/MoCx/MWCNTs nanocomposites with different mass ratios of PtMo were obtained through a molecular self-assembly technology. The structure and morphology of Pt/MoCx/MWCNTs nanocomposites were characterized by several techniques such as XRD, FESEM, XPS, etc. The electrochemical performance and stability of Pt/WCx/MWCNTs electrocatalysts toward EOR were investigated in acid electrolytes. The results show that PtMo exists in the form of alloy. The size of Pt/MoCx nanoparticles is very uniform with an average size of ∼24 nm. The Pt/MoC0.25/MWCNTs exhibits excellent electrocatalytic activities with an electrochemically active surface area of 37.1 m2 g−1, a peak current density of 610.4 mA mgPt−1 and a steady-state current density of 39.8 mA mgPt−1 after 7,200 s, suggesting that the Pt/MoC0.25/MWCNTs is a very promising candidate for application in EOR of DEFCs.
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CATALYSIS LETTERS
·
2022
·Vol. 153
·期 4
·965-977
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IF 2.936
Zhang Tong,Zhao HuaHua,Yang Jian,Zhao Jun,Yan Liang,Chou Lingjun,Song Huanling
Selective hydrogenation of crotonaldehyde to crotyl alcohol over PDA (polydopamine) modified Co 3 O 4 supported Pt catalysts was investigated in liquid phase. The catalysts which contain PDA and Co 3 O 4 lead to the formation of two kinds of interfaces: Pt-PDA and Pt-Co 3 O 4 , which greatly improves the performance in the hydrogenation of crotonaldehyde. TEM results reveal that the Pt nanoparticles of Pt/Co 3 O 4 @PDA have a smaller size and better dispersion than Pt/Co 3 O 4 . XPS, FT-IR and CO-DRIFTs results indicate that the addition of PDA decreases the electron density of Pt which is favor to the hydrogenation of C=O in crotonaldehyde. The characterization results demonstrate that the interaction between Pt and PDA creates new active interfacial sites and the synergy of Pt-PDA and Pt-Co 3 O 4 is responsible for the excellent performance. Graphical Abstract
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
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IF 5.816
Yuanchao Pei,Yajuan Niu,Wanjun Zhang,Yaxin Zhang,Jie Ma,Zhiyong Li
Tunable microstructure of microemulsion self-assembly systems has the prominent application as nanoreactors in reaction processes. Scientific and technological interest in microemulsions derived from the confinement effect of polar or nonpolar domains for hydrophilic/hydrophobic molecules. Benefiting from the tunable nature, ionic liquids-based self-assembly systems have been demonstrated as a versatile platform for catalytic reaction , drug delivery, functional materials fabrication and among others. In this work, ionic liquids microemulsions were designed by using ionic liquids as apolar phase and surfactant . The phase equilibrium and microstructure were studied through phase diagram , conductivity method and dynamic light scattering . Ionic liquids-in-water microemulsions were proposed as nanoreactor for fabrication of nanosized platinum/titanium dioxide composites. The size, morphology and catalytic performance can be tuned by the microemulsion structure through its confinement effect. The hydrolysis of ammonia borane catalyzed by these composites exhibits better catalytic activity with higher turnover frequency and lower activation energy of the reaction. It is believed that the nanoreactors constructed from versatile ionic liquids will provide new guidance in designing advanced scientific applications.
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COLLOIDS AND SURFACES B-BIOINTERFACES
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2021
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IF 5.268
Qianqian Duan,Jialin Wang,Boye Zhang,Xiaoyuan Wang,Juanjuan Xue,Wendong Zhang,Shengbo Sang
As an emerging cancer treatment strategy, photothermal therapy (PTT) is precise, controllable, minimally invasive, low cost and less toxic side effects, thus photothermal transduction agents have been extensively investigated in recent years. Noble metal nanomaterials with unique localized surface plasmon resonance (LSPR) effects are particularly suitable as photothermal transduction agent, but the currently developed precious noble metal nano photothermal transduction agents face serious problems such as complex synthesis process, poor photothermal performance and high biotoxicity. Moreover, the large amount of reactive oxygen species (ROS) produced during PTT treatment could cause irreversible damage to the healthy tissues surrounding the tumor. In this work, we deposited platinum (Pt) on the tips of gold nanorods (AuNRs) to form dumbbell-shaped Au-Pt bimetallic nanorods (AuPtNRs), and functionalized AuPtNRs with biocompatible polydopamine (PDA) to obtain [email protected] With 808 nm laser irradiation, the prepared [email protected] exhibited excellent photothermal stability, and its photothermal conversion efficiency (PCE) reached 81.78%, which was significantly higher than that of AuNRs (52.32%) and AuPtNRs (78.76%). With low cytotoxicity, [email protected] decreased cell viability from 91.12% to 39.36% after PTT on cancer cells in vitro, while significantly reducing intracellular ROS levels generated by heat stress. Therefore, the excellent photothermal properties, high cancer cell killing and ROS scavenging activity of [email protected] in PTT could be an ideal candidate for improving therapeutic efficacy while reducing the risk of toxic side effects due to heat stress-induced ROS formation.
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Nanomaterials
·
2021
·Vol. 11
·期 12
·3266
·
IF 5.076
Yang Li,Yue Lu,Zhaoyu Ma,Lianqing Dong,Xiaofang Jia,Junying Zhang
Graphitic carbon nitride (g-C3N4) has been widely studied as a photocatalyst for the splitting of water to produce hydrogen. In order to solve the problems of limited number of active sites and serious recombination rate of charge-carriers, noble metals are needed as cocatalysts. Here, we selectively anchored Pt nanoparticles (NPs) to specific nitrogen species on the surface of g-C3N4via heat treatment in argon–hydrogen gas mixture, thus achieving g-C3N4photocatalyst anchored by highly dispersed homogeneous Pt NPs with the co-existed metallic Pt0and Pt2+species. The synergistic effect of highly dispersed metallic Pt0and Pt2+species makes the catalyst exhibit excellent photocatalytic performance. Under the full-spectrum solar light irradiation, the photocatalytic hydrogen production rate of the photocatalyst is up to 18.67 mmol·g−1·h−1, which is 5.1 times of the catalyst prepared by non-selective deposition of Pt NPs.Keywords:graphitic carbon nitride;platinum;selective deposition;photocatalytic hydrogen production
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Binbin Zhao,Jieqi Zou,Chen Chen,Qian He,Qiong Tang,Lei Liu,Jinxiang Dong
Pt-WO x -based catalyst has been considered as a promising candidate for the conversion of glycerol to 1,3-propanediol, but the catalytic performance was quite susceptible to the structure and chemical state of WO x species. Herein, we develop a facile approach to construct the single-atom tungsten-doped Al 2 O 3 with a low chemical state through in-situ migration of WO 3 nanoparticles under the H 2 atmosphere. The characterization results demonstrated that the tetrahedral W 5+ could disperse and stabilize the platinum species more effectively, and exhibited stronger interaction with platinum than the octahedral W 6+ species. The enhanced catalytic performance is attributed to the rich oxygen defects on in-situ generated tetrahedral WO x on the catalyst, which facilitated the construction of Pt-WO x interface and strengthened the synergetic effects between them. The analysis of structure-performance correlation revealed that the mono-dispersed tetrahedral W 5+ species [(-O-) 3 W(=O)] played a pivotal role in tuning catalyst acidity and improving the catalytic performance, which assists the adsorption of glycerol and captures H for in-situ formation of Brønsted acid site, and ultimately affected the selectivity toward 1,3-PDO and catalytic activity.
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