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Crystals · 2022 ·Vol. 12 ·期 6 ·778 · IF 2.67

Pt-Modified Interfacial Engineering for Enhanced Photocatalytic Performance of 3D Ordered Macroporous TiO2

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

研究领域: 环境科学 · 材料科学 · 化学工程
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Journal of the American Chemical Society · 2019 · IF 14.695

Ga-Doped and Pt-Loaded Porous TiO2–SiO2 for Photocatalytic Nonoxidative Coupling of Methane

Shiqun Wu,Xianjun Tan,Juying Lei,Haijun Chen,Lingzhi Wang,Jinlong Zhang

Photodriven nonoxidative coupling of CH4 (NOCM) is a potential alternative approach to clean hydrogen and hydrocarbon production. Herein, a Mott–Schottky photocatalyst for NOCM is fabricated by loading Pt nanoclusters on a Ga-doped hierarchical porous TiO2–SiO2 microarray with an anatase framework, which exhibits a CH4 conversion rate of 3.48 μmol g–1 h–1 with 90% selectivity toward C2H6. This activity is 13 times higher than those from microarrays without Pt and Ga. Moreover, a continuous H2 production (36 μmol g–1) with a high CH4 conversion rate of ∼28% can be achieved through a longtime irradiation (32 h). The influence of Ga on the chemical state of a surface oxygen vacancy (Vo) and deposited Pt is investigated through a combination of experimental analysis and first-principles density functional theory calculations. Ga substitutes for the five-coordinated Ti next to Vo, which tends to stabilize the single-electron trapped Vo and reduce the electron transfer from Vo to the adsorbed Pt, resulting in the formation of a higher amount of cationic Pt. The cationic Pt and electron-enriched metallic Pt form a cationic–anionic active pair, which is more efficient for the dissociation of C–H bonds. However, the presence of too much cationic Pt results in more C2+ product with a decrease in the CH4 conversion rate due to the reduced charge-carrier separation efficiency. This study provides deep insight into the effect of the doping/loading strategy on the photocatalytic NOCM reaction and is expected to shed substantial light on future structural design and modulation.

研究领域: 材料科学 · 催化化学 · 理论计算
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FUEL · 2024 · IF 6.7

Enhanced propane dehydrogenation performance using bimetallic-modified GaPt/SiO2-Al2O3 with ultralow-loading Pt

Jingyi Ma,Hui Yuan,Changcheng Liu,Jieguang Wang,Rongxin Zhang,Aizeng Ma

Propane dehydrogenation (PDH) is used to increase propylene production and to produce hydrogen as a by-product. Despite the widespread utilisation of Pt-loaded catalysts in industrial PDH operations, challenges such as excessive noble metal loading and coking persist in the face of rigorous reaction conditions. These hindrances limit to achieving the optimal economic efficiency. In this work, we report a method aimed at reducing Pt loading to only 0.05 wt% through synergistic modification of GaPt catalysts loaded on SiO 2 -Al 2 O 3 supports (i.e. SIRAL) with K and Ce. The resulting catalysts exhibit remarkable stability and elevated activity for propane dehydrogenation. The K + and SiO 2 could modulate the support surface acidity and immobilizes the active tetrahedral Ga 3+ sites, which improves the catalytic performance and reduce coke deposition. Furthermore, the inclusion of Ce decreases the electron density of the Pt species, stabilizing the atomically dispersed Pt and enhances the formation of active Pt sites, which effectively impedes the Pt agglomeration. As a result, the GaPtKCe/SIRAL10 catalyst demonstrates excellent catalytic performance, achieving 47% propane conversion and >96% propylene selectivity, while maintaining notable stability with 0.016 h −1 deactivation rate constant at 580 °C, even without hydrogen co-feed.

研究领域: 化学工程 · 催化材料科学
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Catalysis Science & Technology · 2017 ·Vol. 7 ·期 21 ·5055-5068 · IF 5.773

High selectivity for n-dodecane hydroisomerization over highly siliceous ZSM-22 with low Pt loading

Pengyu Niu,Hongjuan Xi,Jun Ren,Minggui Lin,Qiang Wang,Litao Jia,Bo Hou,Debao Li

Highly siliceous ZSM-22 was synthesized under hydrothermal conditions with ZSM-22 seeds. Characterization by FT-IR and 1H and 29Si NMR spectroscopy confirms that due to the existence of defective sites in the siliceous ZSM-22, acidic silanol groups including vicinal silanol and silanol nests are detected. Acidic silanol groups are considered as the acid sites of siliceous ZSM-22. As a result, siliceous ZSM-22 shows much lower acid site density and lower acid strength than silica–alumina ZSM-22 which contains hydroxyl groups bridging Si and Al as acid sites. In n-dodecane isomerization, Pt/siliceous ZSM-22 shows much higher isomer selectivity than Pt/silica–alumina ZSM-22. Furthermore, a lower loading amount of Pt on siliceous ZSM-22 (about 0.2 wt% Pt) can lead to high isomer selectivity. Owing to the acidic silanol groups and the low acid site density of siliceous ZSM-22, a good balance between metal and acid function in Pt/siliceous ZSM-22 is achieved, which results in a lower allowable Pt loading value and higher isomer selectivity.

研究领域: 催化化学 · 材料科学 · 石油炼制 · 表面化学
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SENSORS AND ACTUATORS B-CHEMICAL · 2017 · IF 5.401

Great enhancement of CH4 sensitivity of SnO2 based nanofibers by heterogeneous sensitization and catalytic effect

Wenbo Lu,Degong Ding,Qingzhong Xue,Yonggang Du,Ya Xiong,Jianqiang Zhang,Xinglong Pan,Wei Xing

In this study, unloaded and Pt-loaded SnO 2 nanofibers (NFs) with 100–150   nm diameters were synthesized by a simple electrospinning technology and then calcined at 600   °C in air. It was observed that the Pt-SnO 2 NFs were comprised of strings of tiny SnO 2 nanoparticles decorated with Pt and PtO nanoparticles, resulting in the formation of PtO/SnO 2 heterojunction and high porosity. And then, we studied the methane (CH 4 ) sensing performance of the sensors fabricated from these NFs and found that 20   mol% Pt-SnO 2 NFs exhibited excellent CH 4 sensing properties over a temperature range of 100–350   °C, for example, the 20   mol% Pt-SnO 2 NFs showed an obvious response of 1.11–1   ppm CH 4 at 350   °C, which was 2 orders of magnitude lower than the minimum detection limit of the current SnO 2 based CH 4 sensors. The great enhancement of the CH 4 sensing properties of Pt-SnO 2 NFs can be understood by the PtO/SnO 2 heterogeneous sensitization and Pt catalytic effect. Our findings present a novel strategy for the application of SnO 2 based NFs in highly effective CH 4 detection.

研究领域: 材料科学 · 传感器技术
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IONICS · 2021 ·Vol. 27 ·期 3 ·1221-1231 · IF 2.817

Facile synthesis of coral-like Pt nanoparticles/MXene (Ti3C2Tx) with efficient hydrogen evolution reaction activity

Li Bishan,Ye Rongkai,Wang Qianyu,Liu Xiaoqing,Fang Pingping,Hu Jianqiang

Exploring efficient catalysts for hydrogen evolution reaction (HER) is one of focus points of energy research. In this work, a series of MXene/Pt- x (wherein, x is the adding amount of 6.2 mM H 2 PtCl 6 solution) nanomaterials were fabricated via a facile synthesis method, in which coral-like Pt nanoparticles (NPs) were deposited on Ti 3 C 2 T x MXene. The Pt-loading amounts on the MXene could be simply controlled by varying the adding amounts of H 2 PtCl 6 , which would influence the sizes of Pt NPs on the MXene. The optimum catalytic activity was obtained on the MXene/Pt-3 with a low overpotential of 302 mV versus reversible hydrogen electrode (RHE) at 10 mA cm −2 , which was about 84 mV less than MXene/Pt-2. The efficiently electrocatalytic HER activity of MXene/Pt- x nanomaterials was due to the electron transfer from MXene to Pt NPs. The HER performance of the MXene/Pt- x nanomaterials was influenced by both Pt-loading amounts and Pt particle sizes. This work expands future applications of MXene-based nanomaterials in clean energy conversion reactions.

研究领域: 材料科学 · 能源研究 · 纳米技术
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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Low Temperature Combustion of VOCs with Enhanced Catalytic Activity Over MnO2 Nanotubes Loaded with Pt and Ni–Fe Spinel

Yaru Wang,Jiaqin He,Xunxun Li,Mengmeng Wang,Yuanbo Zhou,Jun Xiao,Dongyun Chen,Jianmei Lu

MnO2 nanotubes loaded with Pt and Ni–Fe spinel were synthesized using simple hydrothermal and sol–gel techniques. After loading with Ni–Fe spinel, the specific surface area of the material increases 3-fold. This change helped to provide more active sites and facilitated the association between the catalyst and volatile organic compounds (VOCs). X-ray photoelectron spectroscopy determined that the adsorbed oxygen concentrations were all greatly increased after Pt loading, indicating that Pt promoted the adsorption of oxygen and so accelerated the combustion process. The performance of the catalyst after loading with 2 wt % Pt was greatly improved, such that the T90 for benzene decomposition was decreased to 113 °C. In addition, the 2% Pt/2Mn@NFO exhibited excellent low-temperature catalytic activity when reacting with low concentrations of toluene and ethyl acetate. This work therefore demonstrates a viable new approach to the development of Mn-based catalysts for the low temperature catalytic remediation of VOCs.

研究领域: 环境科学 · 催化材料
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NEW JOURNAL OF CHEMISTRY · 2016 ·Vol. 40 ·期 4 ·3225-3232 · IF 3.277

Ultrasonic spray pyrolysis assembly of a TiO2–WO3–Pt multi-heterojunction microsphere photocatalyst using highly crystalline WO3 nanosheets: less is better

Han Zheng,Changhua Wang,Xintong Zhang,Lina Kong,Yingying Li,Yunyu Liu,Yichun Liu

Multi-heterojunctions are more promising than single-heterojunctions in photocatalysis due to the availability of more interfaces between each component. However, photocatalytic activity is highly dependent on the contact mode of individual components. In this work, we assemble TiO2–WO3–Pt multi-heterojunction microspheres using ultrasonic spray pyrolysis and focus on their contact mode governed photocatalytic activity. The results reveal that using highly crystalline WO3 nanosheets as building blocks could particularly enhance the photocatalytic activity of a TiO2/WO3 system toward the degradation of gaseous acetaldehyde and isopropyl alcohol. Furthermore, loading Pt nanoparticles onto WO3 nanosheets could facilitate a more prominent enhancement of activity than that of TiO2/Pt, benefiting from the two-electron reduction of oxygen at the interface of WO3/Pt. Meanwhile, the high crystallinity of WO3 nanosheets allows for a loading amount of Pt as low as 0.04 wt% in the TiO2–WO3–Pt system, which reduces the catalyst cost in comparison with that of the conventional amount of 1 wt%.

CAS / MDL: 18497-13-7
研究领域: 材料科学 · 环境科学 · 催化化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

Heterostructure engineering and ultralow Pt-loaded multicomponent nanocage for efficient electrocatalytic oxygen evolution

Jiongting Yin,Cheng Wang,Kewang Zhang,Dongmei Liu,Zhengying Wu,Shinichi Hata,Rui Yu,Yukihide Shiraishi,Yukou Du

Developing highly efficient electrocatalysts based on appropriate heterojunction engineering and electronic structure modification for the oxygen evolution reaction (OER) has been extensively recognized as an effective approach to increase the efficiency of water splitting. Herein, ultralow Pt-loaded (1 %) NiCoFeP@NiCoFe-PBA hollow nanocages with well-defined heterointerfaces and modified electronic environment are successfully fabricated. As expected, the obtained Pt-NiCoFeP@NiCoFe-PBA exhibits outstanding performance with a low overpotential of 255 mV at 10 mA cm −2 and a small Tafel slope of 57.2 mV dec -1 . More specifically, the highly open three-dimensional structure, exquisite interior voids and abundant surface defects endow Pt-NiCoFeP@NiCoFe-PBA nanocages with more electrochemical active sites. Meanwhile, experimental results and mechanism studies also reveal that the construction of heterogeneous interfaces as well as incorporation of noble metals could readily induce strong synergistic effects and significantly tailor electronic configurations to optimize the binding energy of the intermediates, thereby achieving prominent OER performance.

研究领域: 材料科学 · 电催化 · 能源转换
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Architecturing ultra-stable multi-dimensional MXene/MAX self-supporting electrode anchored with Low-Pt for efficient hydrogen evolution reaction in harsh environments

Li Tian,Tao Hu,Yawen Guo,Peng Ju,Xiujuan Chen,Yueming Li,Xuedong Bai,Guorui Zhao

The design of self-supporting structure is particularly important to improve the stability and electrochemical performance of hydrogen evolution reaction electrode. Here, a facile strategy for building novel ultra-stable 0D-2D-3D integrated self-supporting electrode with high conductivity, sufficient diffusion channels and large reactive surface area was proposed. In the heterostructure, 2D Ti 3 C 2 T x flakes in-situ synthesized on 3D network porous Ti 3 AlC 2 surface which provides the multiple reactive surface areas and aggregation resistance to facilitating 0D ultrafine Pt nanoparticles uniform anchorage. Combined with structural characterization and first-principles calculations revealed that, the highly dispersed ultrafine Pt synergistically coupling strong metal-support interactions creates a unique multifunctional catalytic interface with high stability and atomic utilization efficiency of Pt to promote the HER in acidic and seawater. The resultant self-supporting electrode (support 0.48 wt% Pt) exhibits much superior activity to 10 % commercial Pt/C (loaded on foam nickel) in 0.5 M H 2 SO 4 (55 mV@10 mA cm −2 ) and simulate seawater (196 mV@10 mA cm −2 ) while reducing the Pt usage by 15 times. Meanwhile, the electrode also illustrates outstanding stability under high current densities (100 h@100 mA cm −2 ). This study provides a new design idea for developing integrated self-supporting catalytic electrodes to meet the durability of hydrogen evolution reaction applications in harsh environments.

CAS / MDL: 25322-68-3
研究领域: 材料科学 · 电化学
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Small · 2025 · IF 12.1

Synthesis of Terminal Bifunctional Aliphatic Compounds via Catalytic Oxidation of 1,6-Hexanediol Over Pt-Loaded BiVO4

Zhaoxin Li,Zewen Shen,Haotian Zhang,Chumin Yan,Lisha Yin,Yezi Hu,Guangtong Hai,Guixia Zhao,Xiubing Huang

Terminal bifunctional aliphatic compounds are important intermediates for synthesis of drugs, food additives, polymers, while oxidative conversion from diols in mild conditions and the insight mechanism are rarely investigated. In this work, Pt-loaded BiVO 4 (4%Pt/S-BVO and 4%Pt/H-BVO) is proposed to be utilized for the oxidation of 1,6-hexanediol (1,6-HDO). In dark conditions, the electronic metal-support interactions between Pt and BiVO 4 and abundant oxygen vacancies (OVs) activated C-H and O 2 , leading to the primary oxidation of terminal hydroxyl group of 1,6-HDO. The generated·O 2 − radicals enable further oxidation of aldehyde group to carboxyl group. With illumination, the photo-generated holes promoted oxidation of hydroxyl group to aldehyde group while the increased ·O 2 − radicals promoted the oxidation of aldehyde group to carboxyl group. The introduced heat originated from the photothermal effect and an additional heat source is supposed to boost the mass transfer of molecules and ·O 2 − radicals. In particular, with more abundant OVs and exposed {040} facets, more ·O 2 − radicals, and improved charge separation, 4%Pt/S-BVO exhibit 90% conversion of 1,6-HDO with selectivity of 98.6% to TBACs in 6 h. Those findings highlight the great promise of catalytic organics transformation by integrating solar energy to enhance the reaction efficiency.

CAS / MDL: 107-21-1 13718-26-8
研究领域: 催化化学 · 材料科学 · 有机合成
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Synthesis of Pt-Loaded NiFe-LDH Nanosheets on Wood Veneer for Efficient Gaseous Formaldehyde Degradation

Tailong Cai,Ping Zhang,Xiaoyuan Shen,Erzhuo Huang,Xiaoping Shen,Jiangtao Shi,Zhe Wang,Qingfeng Sun

Traditional methods of removing gaseous formaldehyde are often associated with high energy consumption and secondary pollution. In this study, a new wood veneer-based composite decorated with Pt-loaded NiFe-LDH nanosheets is successfully developed by a hydrothermal reaction and impregnation-chemical reduction. NiFe-LDH nanosheets as an adsorbent can capture formaldehyde molecules through their abundant hydroxyl groups. Pt nanoparticles as catalytic centers are evenly distributed on the surface of NiFe-LDH to excite the O atoms linked to NiFe-LDH and absorbed oxygen, which will further attack the absorbed formaldehyde molecules to generate CO2 and H2O. And the wood veneer not only increases the active area of the catalyst by endowing it with good dispersion but also provides convenient channels for reactants and products. In a simulated dark environment at room temperature, this synthetic wood veneer-based composite exhibits admirable catalytic activity, which can effectively degrade almost all gaseous formaldehyde with the initial concentration of 0.2 mg m–3 in 30 min and maintain a high catalytic activity of ≥97% after 10 cycles. This paper presents a feasible strategy for synthesizing an energy-efficient and ecofriendly wood veneer-based composite for efficient gaseous formaldehyde degradation at room temperature, which may play an important role in indoor air purification as a promising decorative material.

研究领域: 材料科学 · 环境科学
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