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APPLIED CATALYSIS B-ENVIRONMENTAL · 2025 · IF 21.1

Construction of functionalized Pt-O-S bridge on Pt/TiO2 simultaneously enhancing the catalytic activity and sulfur resistance for CO oxidation

Cangpeng Shan,Qinwei Jia,Yan Zhang,Guoshuai Liu,Xinyu Hou,Yunchong Wang,Rui Han,Caixia Liu,Weichao Wang,Qingling Liu

Removing industrial source CO through catalytic oxidation and providing heat for denitrification units have significant economic and environmental benefits. Sulfur poisoning of catalysts is the bottleneck to stabilize the system operation. To overcome this problem, we fabricated sulfate modified Pt/TiO 2 by appropriate NH 4 HSO 4 deposition, which survived in the SO 2 environment with the concentration as high as 1000 ppm SO 2 , and exhibited an outstanding stability with over 90% CO conversion at 200 °C for 500   h under a typical steel sintering flue gas condition. Experimental and theoretical explorations confirmed that the electronic structure of PtO x clusters was optimized through Pt-O-S bridges after sulfate modification. The O 2p band center closer to the Fermi level and the smaller energy difference between Pt 5d and O 2p band centers led to more active lattice oxygen of PtO x clusters. The more stable π back bonding between Pt 5d and CO 2p and weaker hybridization between Pt and the π⁎ (Ssp2-Osp2)2 orbital of SO 2 indicated enhanced CO adsorption while weakened SO 2 adsorption on Pt sites. The above factors simultaneously improved the low-temperature activity and sulfur resistance for CO oxidation over sulfate modified Pt/TiO 2 . This work provides new insights for the design of sulfur-resistant catalysts and the understanding on the effect of sulfates on catalytic activity.

CAS / MDL: 13463-67-7 7803-63-6
研究领域: 催化化学 · 环境化学 · 材料科学 · 化学工程
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ChemistrySelect · 2022 ·Vol. 7 ·期 45 ·e202203391 · IF 2.307

Electrooxidation of Methanol on PANI-CeO2@Pt Catalysts

Qun Xiang,Ruiwen Yan,Guiqi Gao,Shuang Wang

Graphical The PANI-CeO 2 @Pt composites with core-shell structure have been successfully synthesized. Platinum nanoparticles were anchored on the surface of the PANI-CeO 2 materials. The lower potential and higher current density for MOR among the tested PANI@Pt, Pt/C, and CeO 2 @Pt catalysts showed that PANI-CeO 2 @Pt catalyst displayed excellent catalytic performance. This work provided a novel approach to prepare anode catalytic materials and had wide application. Polyaniline (PANI) and Pt were synthesized in sequence by in situ electrochemical deposition on CeO 2 surface to prepare PANI/CeO 2 /Pt ternary composites (PANI-CeO 2 @Pt composites). The electrocatalytic activity of PANI-CeO 2 @Pt composite was measured to 226 mA⋅mg −1 , which was 1.7-, 2.3-, 20-flod as that of CeO 2 @Pt, Pt/C, and PANI@Pt catalyst, respectively. The PANI-CeO 2 @Pt catalyst displayed noticeably the highest activity toward methanol oxidation after the 4000 s among the tested CeO 2 @Pt, Pt/C, and PANI@Pt catalyst. In a CO-stripping experiment, PANI-CeO 2 @Pt composites exhibited better CO tolerance. These results meant that highly dispersed Pt nanoparticles and the oxygen storage capacity of PANI-CeO 2 @Pt contributed to admirable catalytic activities for methanol oxidation reaction (MOR).

研究领域: 材料科学 · 电化学
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Materials · 2014 ·Vol. 7 ·期 12 ·8105-8130 · IF 1.879

Metal Phosphate-Supported Pt Catalysts for CO Oxidation

Xiaoshuang Qian,Hongmei Qin,Tao Meng,Yi Lin,Zhen Ma

Oxides (such as SiO2, TiO2, ZrO2, Al2O3, Fe2O3, CeO2) have often been used to prepare supported Pt catalysts for CO oxidation and other reactions, whereas metal phosphate-supported Pt catalysts for CO oxidation were rarely reported. Metal phosphates are a family of metal salts with high thermal stability and acid-base properties. Hydroxyapatite (Ca10(PO4)6(OH)2, denoted as Ca-P-O here) also has rich hydroxyls. Here we report a series of metal phosphate-supported Pt (Pt/M-P-O, M = Mg, Al, Ca, Fe, Co, Zn, La) catalysts for CO oxidation. Pt/Ca-P-O shows the highest activity. Relevant characterization was conducted using N2adsorption-desorption, inductively coupled plasma (ICP) atomic emission spectroscopy, X-ray diffraction (XRD), transmission electron microscopy (TEM), CO2temperature-programmed desorption (CO2-TPD), X-ray photoelectron spectroscopy (XPS), and H2temperature-programmed reduction (H2-TPR). This work furnishes a new catalyst system for CO oxidation and other possible reactions.Keywords:metal phosphate;hydroxyapatite;Pt catalyst;CO oxidation

CAS / MDL: 7784-30-7
研究领域: 催化化学 · 材料科学
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SENSORS AND ACTUATORS B-CHEMICAL · 2023 · IF 8.4

Pt-modified BiVO4 nanosheets for enhanced acetone sensing

Yanwei Xiao,Shuhe Hu,Yuanyuan Liu,Ao Zhang,Zhen Yao,Ye Tian,Huiling Li,Yang Ning,Feng Li,Fengdong Qu,Dong Yao,Hao Zhang

Two-dimensional (2D) BiVO 4 nanosheets (NSs), featuring distinctive chemical properties and dangling-bond-rich surfaces, are promising for developing high-performance gas sensors. However, the previously reported 2D BiVO 4 NSs-based devices suffer from a low responsivity and poor selectivity. Here, catalytic metal (Pt) nanoparticles (NPs) are functionalized on the surface of BiVO 4 NSs to improve the sensing ability. Comparative investigations verify the significant enhancement in acetone sensing after Pt modification. The Pt NPs-loaded BiVO 4 exhibits a response of 12.5–100 ppm acetone, which is 3.2 times higher than that of pure BiVO 4 sensor. Besides, the Pt-BiVO 4 sensor possesses better selectivity and lower detection limit. From both the experimental results and density functional theory (DFT) calculation, the effects of Pt modification are elucidated as a synergy of chemical and electronic sensitization. The loading of Pt benefits the thickening of electron depletion layer , and accumulating and activating the acetone molecules, which accelerate the reaction between acetone and chemisorbed oxygen species, resulting in enhanced sensing performance. This work gives deep insights into the effects of noble metal modification on metal oxide-based sensing material and could serve as a guideline for further designing novel high-performance sensing materials.

研究领域: 材料科学 · 传感器技术
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NEW JOURNAL OF CHEMISTRY · 2021 ·Vol. 45 ·期 23 ·10315-10324 · IF 3.591

A cathodic photocorrosion-assisted strategy to construct a CdS/Pt heterojunction photocatalyst for enhanced photocatalytic hydrogen evolution

Jianming Fan,Jinhua Xiong,Dayue Liu,Yuanping Tang,Song He,Zhibiao Hu

A novel strategy was developed to fabricate a CdS/Pt photocatalyst (defined as CdS/w%Pt-PAR) via the cathodic photocorrosion effect of CdS. A tentative mechanism for Pt deposition on CdS via the cathodic photocorrosion effect was proposed, based on a series of electrochemical characterization methods, such as cyclic voltammetry and Mott-Schottky tests. Transmission electron microscopy verified that Pt was grafted on the CdS surface via a heterojunction. Moreover, a strong interaction between Pt and CdS was further confirmed by X-ray photoelectron spectroscopy. The optimal photocatalytic H2 evolution rate of CdS/2%Pt-PAR was 1086.1 μmol h−1, 6.4 and 2.6 fold higher than that of the reference samples synthesized by traditional photodeposition (CdS/2%Pt-PD) and chemical reduction (CdS/2%Pt-CR) methods, respectively. Linear sweep voltammetry and fluorescence experiments verified that CdS/2%Pt-PAR has a lower H2 evolution overpotential and faster separation of photogenerated carriers, respectively, compared with CdS/2%Pt-PD and CdS/2%Pt-CR. This work paves a new route for fabricating CdS/metal photocatalysts with highly efficient and stable photocatalytic H2 evolution activity.

CAS / MDL: 1306-23-6
研究领域: 材料科学 · 能源科学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2017 · IF 3.582

Optimizing the hydrogen evolution reaction by shrinking Pt amount in Pt-Ag/SiNW nanocomposites

Wen Shen,Bin Wu,Fan Liao,Binbin Jiang,Mingwang Shao

In recent years, platinum-based catalysts are the most promising candidates for hydrogen evolution reaction (HER). Decrease of the Pt usage is an effective way to obtain low-cost hydrogen production. In order to achieve this goal, we synthesized Pt-Ag/SiNW composites with different dosages of Pt, using inexpensive Ag as a co-catalyst and SiNWs as carriers, and tested their catalytic performance in HER. The results showed that the optimal composition of Pt: Ag: Si = 4.1: 21.5: 74.4 in mass ratio. With such a low amount of Pt, the Pt-Ag/SiNW catalyst exhibited exciting HER performance, whose turnover frequency is 6.3H 2 Pt −1 s −1 at −0.2 V vs. RHE, 2.7 times as large as that of 40 wt% Pt/C. This design greatly increased the utilization ratio of Pt, which may open a new way for preparation of other Pt-based catalysts.

CAS / MDL: 18497-13-7 7761-88-8
研究领域: 材料科学 · 能源化学
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JOURNAL OF CATALYSIS · 2020 · IF 7.888

Atomically dispersed Ptn+ species as highly active sites in Pt/In2O3 catalysts for methanol synthesis from CO2 hydrogenation

Zhe Han,Chizhou Tang,Jijie Wang,Landong Li,Can Li

Hydrogenation of CO 2 into methanol using the H 2 produced from renewable energy is a promising way for carbon capture and utilization. Therefore, the methanol synthesis catalysts with high methanol selectivity are highly desired. In this work, we found that the methanol selectivity of In 2 O 3 catalyst can be significantly enhanced by introducing a small amount of Pt. Methanol selectivity can be increased from 72.2% (In 2 O 3 ) to 91.1% (0.58 wt.% Pt/In 2 O 3 ) at 220 °C. The introduced Pt atoms are doped into the In 2 O 3 , forming atomically dispersed Pt n+ species, most of which are stable under working conditions. It is proposed that the atomically dispersed Pt n+ species are responsible for the enhanced methanol selectivity, while Pt nanoparticles on In 2 O 3 mainly boost the reverse water-gas shift reaction (CO 2  + H 2  → CO + H 2 O).

研究领域: 催化 · 化学工程 · 可再生能源
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AICHE JOURNAL · 2023 ·Vol. 69 ·期 9 ·e18149 · IF 3.7

Taming Pt 5d state occupancy via Pt?O?Mn electronic linkage for enhanced dehydrogenation activity

Yongxiao Tuo,Ying Meng,Qing Lu,Qing Wang,Furong Jia,Yan Zhou,Xiang Feng,Jun Zhang,Xuezhi Duan,De Chen

The enhancement of catalytic activity is always limited by the dilemma in activation and desorption due to Sabatier principle. Locating the Sabatier optimum by manipulating catalyst electronic structure has been a long-standing challenge in heterogeneous catalysis. Herein, we presented a generic strategy to continuously tailor the Pt 5d state occupancy via tuning the Pt  O  Mn electronic linkage over Al 2 O 3 -confined MnO x islands, aiming at accommodating the C  H cleavage and product desorption capabilities in dehydrogenation of liquid organic hydrogen carriers (monocyclic/bicyclic hydrides). Rising Mn valence can decrease the Pt 5d state occupancy through more electron transfer from Pt 5d to O 2p due to the strong π-donation of O 2p to Mn 3d. This will lead to the lower initial C  H activation energy barrier while higher product desorption energy barrier. An intermediate Pt 5d filling of ~8.4 in Pt  Mn 2 O 3 /Al 2 O 3 enables the balanced level of product desorption and C  H activation, thus ensuring a superior dehydrogenation activity. The electron structure-adsorption-performance modulation mechanism described herein provides a benchmark to locate the Sabatier optimum for the metal catalyst design.

研究领域: 多相催化 · 材料科学 · 化学工程 · 物理化学
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ACS Applied Nano Materials · 2022 · IF 6.14

Modulating Pt Interaction in Au@Pt Nanoparticle/WO3 Photocatalysts for Enhanced Production of Peroxodisulphate

Zeai Huang,Yaolin Chen,Jundao Wu,Wenwen Xie,Xiaoting He,Minzhi Ma,Kazuhiro Sayama,Ying Zhou

Production of peroxodisulphate (S2O82–) on powdered photocatalysts is a promising way to obtain high-value-added chemicals using solar energy; however, it is still suffering from low efficiency. In the present work, we fabricated bimetallic Au core and Pt shell nanoparticle-loaded WO3 (Au@Pt/WO3) photocatalyst for enhanced production of S2O82–, which is 1.7 times that of Pt nanoparticle-loaded WO3 (Pt/WO3), and was reported to be the best catalyst for S2O82– production. A further study demonstrated that the electronic interaction of Pt was successfully modulated by the core–shell nanoparticle architecture, and the core–shell nanoparticle structure between Au and Pt improved the formation of the surface chemical state of Pt to be metallic Pt, proposed as the active site for oxygen reduction. Besides, the core–shell nanoparticle structure also exposed a large amount of Pt on the surface of the substrate. As a result, Au@Pt/WO3 showed significantly enhanced photocatalytic activity of S2O82– with a quantum efficiency of 5.2% at 420 nm, whereas Pt–Au bimetallic alloy nanoparticle-loaded WO3 with a large amount of surface PtOx and exposed both Au and Pt on the surface showed very low activity. This work provides insights into the bimetallic Pt nanoparticle-loaded WO3 for enhanced photocatalytic activity.

研究领域: 材料科学 · 环境科学 · 化学
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Catalysts · 2021 ·Vol. 11 ·期 2 ·174 · IF 4.146

Synthesis of Au or Pt@Perovskite Nanocrystals via Interfacial Photoreduction

Jing Zhang,Li Wang,Wenwen Liu,Mengsha Cao,Jing Zhang,Ningyi Yuan,Shuai Zhang,Zhongze Gu

The surface modification of perovskite nanocrystals (NCs) (i.e., their decoration with noble metals) holds great promise with respect to the tailoring of their properties but has remained a challenge because perovskite NCs are extremely sensitive to water and alcohols. In this study, Au or Pt@CsPbBr3NCs were successfully synthesized by photoreduction at the water/hexane interface. First, Cs4PbBr6NCs were synthesized through the hot-injection method. Then, Cs4PbBr6was transformed into CsPbBr3and subjected to noble metal modification, both at the interface. The synthesized CsPbBr3NCs exhibited a cubic perovskite phase and had an average size of approximately 13.5 nm. The deposited Au and Pt nanoparticles were crystalline, with a face-centered cubic lattice and average diameters of approximately 3.9 and 4.4 nm, respectively. The noble metal modification process had almost no effect on the steady-state photoluminescence (PL) emission wavelength but affected the charge-recombination kinetics of the CsPbBr3NCs. Time-resolved PL decay spectral analysis indicated that the fluorescence lifetimes of the Au and Pt@CsPbBr3NCs were shorter than those of the pure CsPbBr3NCs, probably owing to the quenching of the free charges because of electron transfer from the perovskite to the noble metal nanoparticles.Keywords:perovskite nanocrystals;noble metal;interface;photoreduction

研究领域: 材料科学 · 化学
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Catalysis Science & Technology · 2017 ·Vol. 7 ·期 13 ·2717-2728 · IF 5.773

Mechanistic insights into complete hydrogenation of 1,3-butadiene over Pt/SiO2: effect of Pt dispersion and kinetic analysis

Chaoquan Hu,Jiahan Sun,Dongjuan Kang,Qingshan Zhu,Yafeng Yang

Gas-phase hydrogenation of 1,3-butadiene was investigated over Pt/SiO2 catalysts with the aim of understanding the complete hydrogenation of dienes. The measurements focused on the effect of Pt dispersion on the product distribution and the kinetics of n-butane formation. Under the investigated conditions with an excess of hydrogen, the selectivity to n-butane sharply decreased from 41.6% to less than 3% at a 1,3-butadiene conversion of ∼10% when the average Pt particle size increased from 3.9 to 22 nm. Correspondingly, the apparent activation energy for n-butane formation was measured to increase by about 2.7 times. In situ diffuse reflectance infrared Fourier transform (DRIFT) observations via alternating 1,3-butadiene and hydrogen feeds over the catalysts demonstrated that 1-butene was the major reaction intermediate in the process of 1,3-butadiene hydrogenation. By analysis of the kinetic data using the Horiuti–Polanyi mechanism with 1-butene as the intermediate, different reactivities of hydrogen on the catalysts towards CC bond hydrogenation were proposed to understand the variation of the selectivity to n-butane with Pt dispersion. This viewpoint was further supported by DFT calculation of 1-butene hydrogenation with hydrogen at different sites on the Pt(111) surface.

CAS / MDL: 18496-40-7
研究领域: 催化化学 · 材料科学 · 表面科学
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CATALYSIS TODAY · 2020 · IF 5.825

Basic carrier promoted Pt-catalyzed hydrogenolysis of alkaline lignin

Jian Zhang,Zerui Su,Zhiyi Wu,Pingzhou Wang,Feng-Shou Xiao

Catalytic hydrogenolysis of lignin to produce arene monomers is promising for efficient utilization of lignocellulose. The acidic carrier supported metal nanoparticles exhibit excellent catalytic performance, while basic carrier was not often used. In this study, a basic hydroxyapatite supported Pt nanoparticles (Pt/HAP-3) were developed for the catalytic hydrogenolysis of alkaline lignin, achieving 15.1 % monomer yield. Characterizations of the catalysts and investigation on the basic sites show that high monomer yield is resulted from the synergy of suitable metal nanoparticles and sufficient basic sites of the carrier. This work might be helpful for preparation of efficient catalysts for the hydrogenolysis of lignin in the future.

研究领域: 化学工程 · 催化科学
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