APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Mingshuo Tian,Zhiwei Huang,Jiangwei Ni,Wen Chen,Qiqi Zhou,Huazhen Shen,Xiaomin Wu,Huawang Zhao,Guohua Jing
The elucidation of active sites in Pt-based catalysts for benzene combustion has been a long-standing challenge, hindering the rational design of such catalysts. We have successfully pinpointed the active sites to the perimeters of Pt nanoparticles, deliberately excluding corner atoms. This achievement stems from a comprehensive approach, encompassing controlled synthesis of Pt nanocrystal size and morphology, advanced spectroscopic characterization, and detailed geometrical model analysis. We synthesized well-defined truncated hexahedral Pt nanoparticles with diameters (d) ranging from 2.2 to 6.6 nm. Notably, the turnover frequency (TOF) of our Pt/TiO 2 catalyst correlates inversely with the nanoparticle diameter, following a d -1.09±0.11 trend. This correlation matches the model-predicted perimeter-to-diameter ratio (excluding corners) with a d -1.01±0.09 exponent, confirming the location of the active sites. Further support comes from X-ray photoelectron spectroscopy and experiments using different support materials, which underscore the high activity at the Pt/TiO 2 interface. A crucial H 2 treatment step encapsulating the Pt nanoparticles by TiO x excludes both surface areas and corners as contributing active sites. The 0.7 % Pt/TiO 2 catalyst also demonstrated remarkable stability under testing conditions. In situ FTIR analysis provided insight into the stepwise mechanism of benzene combustion, revealing intermediate species and their transformation pathways. By finely tuning the geometry of Pt nanoparticles and correlating TOF with specific surface sites, our research highlights the perimeters of Pt atoms as the prime active sites for benzene combustion. These results contribute significantly to the field, offering a strategic approach to designing efficient catalysts for VOC elimination, with implications for both environmental protection and the advancement of catalytic science.
研究领域:
催化科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Jin Zhang,Zixin Chen,Zerong Bian,Huixian Ma,Kun Liang,Meiling Liu,Xincheng Li,Yunwei Wang,Ruiyi Wang,Zhanfeng Zheng
Anion modification offers a promising approach for the specific conversion of reaction substrates in catalytic processes. In this study, we synthesized Pt-based metal nanocatalysts on a TiO 2 support and modified them with PO 4 3- anions, thereby achieving a complete shift in CO 2 hydrogenation products from CO to CH 4 . The original Pt-P 0 /TiO 2 catalyst exhibited a low degree of CO 2 conversion (4.5%), and the hydrogenation products comprised primarily CO. In contrast, the Pt-P 3 /TiO 2 catalyst modified with PO 4 3- anions exhibited a 5.2-fold increase in the degree of CO 2 conversion (23.2%) and excellent methane selectivity. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and CO-temperature-programmed desorption (TPD) characterization revealed distinct reaction pathways. Notably, the desorption of CO intermediates predominated for the Pt-P 0 /TiO 2 catalyst, whereas further hydrogenation of CO prevailed on the surface of the Pt-P 3 /TiO 2 catalyst. The results of X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) calculations indicated that PO 4 3- anions adsorbed preferentially at Pt metal sites, modulating the surface electronic properties of the Pt metal and its adsorption and desorption behaviours towards CO, thereby increasing the CO 2 conversion efficiency and causing a shift in hydrogenation products. This work provide valuable insights for designing high-performance catalysts for ensuring sustainable CO 2 conversion.
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2026
·
IF 18.1
Zhang Chi,Tang Wenxiang,Li Xiangyang,Zhang Chi,Zou Zongpeng,Zhu Yifeng,Tang Shengwei,Chen Yunfa,Gao Pu-Xian
Design of active but stable interfaces in supported metal catalysts represents an emerging research theme lately, given its critical importance for tailoring and enabling selectivity and efficiency of heterogeneous reactions. Herein, we report a generic sunlight-driven epitaxial growth strategy to engineer catalytically active interfacial perimeters defined by subnanometric Pt dispersed on TiO 2 nanoparticle supports. Such interfacial perimeters are populated with a unique type of Pt 4+ -O-Ti 3+ reactive sites, resulting in much more efficient and robust CO oxidation than most supported Pt catalysts reported so far. These subnanometric PtO x -TiO 2 interfacial structures are found to dynamically evolve during CO oxidation, adaptively optimizing their adsorption behaviors toward reactants and SO 2 . Combined with the activated interfacial lattice oxygen species via the electronic metal-support interaction effect, the Mars-van Krevelen pathway is activated at low temperature to oxidize CO at high conversion efficiency. The sunlight-driven synthetic strategy is successfully extended to other metal catalysts supported by metal oxide and perovskite materials, offering a new paradigm for designing adaptive catalysts toward a variety of heterogeneous catalytic reactions.
✓ 已验证
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Yuqin Lu,Hua Deng,Xueshan Zhang,Jianguo Ding,Sijia Bai,Lian Wang,Hong He
The inhibitory interactions among various volatile organic compounds (VOCs) during combustion in industrial exhaust gases pose a significant challenge for catalytic technologies, primarily due to a lack of effective approaches to counter these adverse effects. The interaction between Pt and TiO2 was readily tuned through hydrogen reduction of the TiO2 matrix (Pt/TiO2-800), which ultimately transformed the inhibitory effect into a synergistic effect in a toluene–acetone mixture. Optimal catalytic activity was achieved at 0.6 wt % Pt loading, with 0.6Pt/TiO2-800 lowering reaction temperatures by 21 °C for toluene and 24 °C for acetone in mixed VOC oxidation. Characterization reveals that Pt/TiO2-800 possesses abundant oxygen vacancy clusters, enhancing TiO2-Pt electron transfer, diversifying Pt nanoparticle sizes, stabilizing low-valent Pt species, and improving oxidative capacity. DFT calculations further underscore the role of oxygen vacancy in modulating the Pt electronic environment and enhancing defect-enhanced adsorption. This work advances Pt-TiO2 interaction understanding and offers an effective catalyst for VOCs abatement, addressing inhibitory effects in mixed VOCs systems.
研究领域:
催化化学
·
环境化学
·
材料科学
·
多相催化
·
污染控制
✓ 已验证
DOI
PubMed
高影响因子
CATALYSIS LETTERS
·
2018
·Vol. 148
·期 8
·2418-2431
·
IF 2.911
Sun Rong,Huang Wan,Zhang Qian,Hong Jun-ming
Abstract This study developed nitrogen-doped graphene/Pt/TiO 2 (N-GN/Pt/TiO 2 ) as anode to effectively degrade aminophenol (APAP) in electrocatalytic process. Due to the different physicochemical properties of graphene with various N species loading, the efficiency of catalysts was novelty discussed. The morphology, N-doped content/species, and the graphene defects of the catalyst were analyzed by TEM, FTIR, XPS, EA, and Raman spectroscopy. The results show that the doping morphology of the N atoms gradually shifted from pyridinic N and pyrrolic N to graphitic N with increased hydrothermal time, in order to decrease the defect degrees and redox activity. However, the conductivity of material increased with the graphitic N generation. The best APAP degradation efficiency (100% with 20 mA, 1 g/L NaCl, and initial pH 3.0) can be achieved with 1.5-N-GN/Pt/TiO 2 (mainly pyridinic N and pyrrolic N doping). A detailed investigation was conducted to determine the oxidation intermediates of APAP using GC-MS analysis. Finally, a possible degradation pathway was proposed. Graphical Abstract
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
RSC Advances
·
2012
·Vol. 2
·期 32
·12378-12383
·
IF 0
Xuefeng Hu,Huanhuan Ji,Lei Wu
Pure and Pt nanoparticle-modified rutile TiO2 were synthesized via hydrolysis of TiCl4 in the absence or presence of Pt nanoparticles. HRTEM, XRD, and SEM were used to characterize the structure of the prepared catalysts. The resulting modified TiO2 catalysts show extended visible light absorbance. Photodegradation of 2,4,6-trichlorophenol (2,4,6-TCP) over these photocatalysts was investigated under visible light illumination. The Pt nanoparticles facilitate the separation of photogenerated electron–hole pairs at low Pt content, then enhances the photodegradation rate of 2,4,6-TCP. 0.18Pt–TiO2 achieved the best photocatalytic activity among the tested catalysts. It was found that singlet oxygen rather than ˙OH acts as the main oxidative species for the degradation of 2,4,6-TCP according to the experimental results. The degradation intermediates of 2,4,6-TCP were identified and the degradation pathway was proposed. Pt nanoparticles on TiO2 significantly enhance O2 adsorption and the formation of ˙O2−. The rutile surface is a favorable condition for stabilizing ˙O2−. These properties of the Pt nanoparticle-modified rutile TiO2 facilitate the formation of 1O2via the reaction of superoxide anions with holes.
研究领域:
环境科学
·
材料科学
·
光催化技术
✓ 已验证
产品关联
DOI
MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Na Sun,Jiaojiao Song,Qingmei Tao,Erjie Kan,Long Kuai
Photocatalysis utilized solar energy with metal oxide semiconductors has been considered as one of the attractive green routes for organics’ conversion. The construction of high-density co-catalytic sites is essential for the surface reaction kinetics . In this work, a high-efficiency mesoporous TiO 2 decorated with single atomic Pt loading of 1 at% (2.1 wt%) had been successfully achieved. The high specific surface area of mesoporous TiO 2 affords adequate physical surface for the resident of atomic Pt, thus stabilizing a high areal density of single-atom reaction sites. The optimized single-atom Pt/TiO 2 revealed a performance of 4.1 mmol/h/g cat for photocatalytic oxidation of benzyl alcohol under visible light irradiation that is 3.8 folds than that of Pt-modified commercial TiO 2 photocatalysts . The reactivity will further enhance after the introduction of plasmonic Au nanoparticles and the finally sample (1 at % Pt-0.075 at % Au)/TiO 2 -MP exhibited salient activity (4.5 mmol/h/g cat ) and stability. This work paves a potential way to boost the performance of metal oxide semiconductors for green photocatalytic conversion of organics.
研究领域:
材料科学
·
光催化化学
✓ 已验证
DOI
高影响因子
Catalysts
·
2026
·Vol. 16
·期 7
·620
·
IF 4.5
Li Fang,Yuxian Jiang,Xueyang Jiang,Qin Zhang,Sihui Suo,Chenhui Zhao,Jiayu Song,Jiancong Liu
Oxygen vacancies are a key factor determining the efficiency of the CO2hydrogenation reaction and play a crucial role in CO2adsorption and activation. However, effectively regulating the concentration of oxygen vacancies to enhance the performance of the light-driven reverse water gas shift (RWGS) reaction remains a challenge. To address this, this study successfully developed Pt/TiO2catalysts with varying oxygen vacancy concentrations by controlling the morphology of TiO2. Structural characterization results indicate that, compared to Pt/TiO2-NR, Pt/TiO2-NB exhibits a higher oxygen vacancy (OV) concentration and greater CO2absorption. Catalytic performance evaluation results showed that under an irradiance of 2.5 W/cm2, the CO production rates of the Pt/TiO2-NB catalyst reached 57.03 mol·gPt−1·h−1. Furthermore, the catalyst maintained excellent catalytic stability during 45 h of continuous operation, demonstrating good potential for practical applications.
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2026
·
IF 17.2
Yiwei Zhao,Zuhang Jin,Cheng Tao,Rui Du,Yongzheng Shi,Chao Zhang
The synthesis of KA oil (a cyclohexanone-cyclohexanol mixture) from guaiacol through mild electrocatalytic approach represents a sustainable strategy for biomass valorization. Herein, we report the electrocatalytic conversion of guaiacol to KA oil over the reduced Pt/TiO 2 catalysts. The TiO 2 -induced hydrogen spillover effect facilitates strategic modulation of H ads (H*) coverage on Pt surfaces, thereby effectively suppressing competitive aromatic ring hydrogenation and excessive hydrogen evolution reactions. Comparative studies of electrocatalysis and thermocatalysis have demonstrated that Pt active sites serve as the dominant catalytic centers. However, H spillover significantly influences reactivity and selectivity, particularly in the electrocatalytic pathways. The electrocatalytic system demonstrates preferential C–O bond cleavage with KA oil selectivity around 70%. This work provides valuable insights into the regulation of metal-support interactions in the design of electrocatalysts.
✓ 已验证
产品关联
DOI
高影响因子
SENSORS
·
2025
·Vol. 25
·期 10
·3195
·
IF 3.5
Cuiyan Han,Ziao Wang,Jiahong Cui,Shuqi Liu,Liu Yang,Yang Fu,Baolin Zhu,Cheng Guo
This article presents an integrated strategy that couples high-efficiency photocatalytic degradation with low-cost, rapid detection to overcome the main drawbacks of conventional TiO2-based photocatalysts, including a weak visible-light response, rapid charge–carrier recombination, and reliance on expensive instrumentation for dye concentration detection. Platinum-decorated TiO2(Pt/TiO2) was prepared by photoreduction deposition, and systematic characterization confirmed the successful loading of zero-valent Pt nanoparticles onto the TiO2surface, significantly improving charge separation and extending absorption into the visible region. Methylene blue degradation was quantified under ultraviolet (UV) and simulated sunlight; radical-scavenging tests clarified the reaction pathway. In parallel, smartphone images of the reaction mixture were processed in ImageJto extract red–green–blue (RGB) values, which were related to dye concentration through a partial least-squares (PLS) model validated against reference UV–Vis data. Pt/TiO2removed 95.0% of methylene blue within 20 min of UV irradiation and 90.2% within 160 min of simulated sunlight—31.8% and 19.1% faster, respectively, than pristine TiO2. The RGB-based PLS model achieved a coefficient of determination (R2) of 0.961 for the prediction set. By integrating photocatalysis with smartphone-based colorimetry, the proposed method enables rapid monitoring of organic dyes concentration, providing an intelligent and economical platform for industrial wastewater treatment.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Yang Zou,Xue Li,Yongqi Zhao,Xiaolong Liu,Shaohua Xie,Fudong Liu,Tingyu Zhu
Defect engineering has attracted great attention due to its important role in promoting metal dispersion and regulating catalytic performance. In this study, a gentle method for stabilizing metal single atoms and adjusting the metal coordination environment was proposed, wherein the chemical etching of a Ti–Si oxide composite by NaOH was employed to construct a defect structure. As a conceptual proof, a defective catalyst loaded with 0.1 wt % Pt was synthesized, which exhibited a complete CO oxidation temperature of 200 °C, a significant 70 °C decrease compared to the conventional catalyst. Characterization and theoretical calculations confirmed that Pt existed as single atoms on the defective catalyst, and O2 was adsorbed and activated at Ti3+ defect sites. Notably, the CO oxidation followed the Mars-van Krevelen (MvK) mechanism, resulting in a remarkably low oxygen activation energy barrier of 0.38 eV on the defective catalyst, significantly lower than that on the conventional catalyst (2.48 eV), consistent with its enhanced low-temperature activity. This work provides a promising strategy for the design of efficient and stable low-load noble metal catalysts on oxide-based supports.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Chenghao Yao,Jinbiao Huang,Can Yang,Weiwei Deng,Lei Li,Zhan Lin
Photo-thermal catalysis which interplay the heat and light-induced effects have drawn broad attention owing to their synergistic effect to extend the capability of chemical transformation. Here, the effect of heat and/or light on methanol decomposition has been clarified. On Pt/TiO 2 , light irradiation activates the TiO 2 and enhance the absorption and the oxidation of intermediates. The main intermediate under PTC condition is formaldehyde, which is the same to TC condition rather than methyl formate under PC condition. Differences CO absorption site correlates with the key intermediates under PC and TC/PTC conditions. Light and heat display their strengths in a synergistic manner, optimizing the activity to promote efficient catalytic processes which is verified to be photo-assisted thermal catalysis. This work offers detailed mechanistic understanding of the surface species and paves the way for an educated microkinetic modeling approach under photo and/or thermal condition over oxide-supported metal catalysts.
研究领域:
催化化学
·
材料科学
·
物理化学
·
表面科学
·
能量转换
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）