PROCEEDINGS OF THE COMBUSTION INSTITUTE
·
2022
·
IF 6.535
Xing Yuan,Chaohe Zheng,Zuwei Xu,Qinghua Yang,Tiantian Zhang,Xi Luo,Haibo Zhao
Photothermocatalytic oxidation is an environmentally-friendly, low-temperature, and high-efficient method to remove the air pollutant. Yet, the lack of active, inexpensive, and superior stability catalysts has greatly limited its extensive utilization. In this work, the effect of single-atom Pt loading on TiO 2 support has been theoretically and experimentally studied to improve photothermocatalytic performance for the toluene combustion through flame spray pyrolysis (FSP). Pt loading can play two crucial roles into TiO 2 optimization: (1) The low-valence Pt cation incorporated into TiO 2 lattice is dramatically responsible for the anatase-rutile transformation (ART) and formation of sufficient oxygen vacancies ; (2) Introducing the defect energy level and Pt-3d orbitals remarkably promote the charge separation efficiency of single-atom catalysts. Moreover, the existence of single-atom Pt nanoparticles can signally boost the activity of surface adsorbed and lattice oxygen, as well as substantially reduce the oxygen vacancy formation energy. Thus, the toluene removal under light irradiation reaches 90% conversion below 160 °C and is maximally 18 °C lower than that under only thermocatalytic oxidation. It is attributed to larger specific surface area (SSA), outstanding low-temperature reducibility, extremely dispersed hybrid PtO x , more surface active oxygen, and higher mobility of bulk oxygen. Interestingly, when the oxygen-fuel equivalent ratio φ distinctly increases by shifting precursor solvent from xylene to ethanol, the photothermocatalytic property of toluene can be remarkably enhanced on single-atom Pt catalysts. It is due to the higher Pt dispersion resulting from more intense burning and drastic turbulent mixing, as well as the superior ratio of the metallic Pt active sites originating from higher flame temperature. Eventually, the rate-determining step of C 7 H 8 combustion on Pt/TiO 2 and Cu/TiO 2 slab are all the C C bond fracture of maleic anhydride to form acetic anhydride species, with the energy barriers of 112.03 and 188.74 kJ/mol, respectively.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Peng Liu,Yahao Zhao,Wen Liu,Furong Ye,Hui Lv,Zhuo Peng,Changcun Han,Xinguo Ma,Jiayi Tian,Difu Zhan,Qian Fu,Yizhong Huang
Solar photocatalytic hydrogen production shows promise in addressing global energy and environmental concerns. The limited efficiency of photocatalysts is mainly due to ineffective separation and transfer of photogenerated charges. To improve this, we enhance the TiO 2 –Ti 3 C 2 heterojunction by in-situ oxidation through interfacial engineering , resulting in a more compact composition . Subsequently, we anchor single-atom Pt at the TiO 2 –Ti 3 C 2 interface through photo-Ti 3 C 2 reduction. The in-situ growth of TiO 2 on Ti 3 C 2 introduces an interfacial driving force for carrier separation and provides a channel for electron transfer from TiO 2 to Ti 3 C 2 . This further facilitates transfer onto Pt, shortening the migration distance and enhancing the photocatalytic efficiency. The best Pt/TiO 2 –Ti 3 C 2 composite demonstrates an impressive hydrogen precipitation efficiency of 767 μmol g −1 h −1 , surpassing TiO 2 and Pt/TiO 2 by factors of 12 times and 1.46 times, respectively. Furthermore, we developed a higher efficiency photocatalyst using the molten salt method to avoid the risks associated with conventional hydrofluoric acid etching. This research opens up new possibilities for the preparation of MXenes interface-modified catalysts, offering a valuable avenue for future exploration in the field.
研究领域:
材料科学
·
能源与环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2022
·
IF 13.7
Yongjun Ji,Shaomian Liu,Shaojia Song,Wenqing Xu,Liang Li,Yu Zhang,Wenxing Chen,Huifang Li,Jingang Jiang,Tingyu Zhu,Zhenxing Li,Ziyi Zhong,Dingsheng Wang,Guangwen Xu,Fabing Su
Pt-based catalysts are promising for the selective catalytic reduction of NOx by CO (CO-SCR), but some technical issues hinder their practical application, including the high Pt loading needed, high reduction temperature, and the low tolerance toward SO2. Here, we report a novel Pt catalyst for CO-SCR, which has negatively charged single-atom Pt embedded on CuO squares, and the latter is supported on CoAlO nanosheets. This Pt–CuO/CoAlO catalyst with an ultra-low Pt loading (0.02 wt %) exhibited 91% NO conversion and 80% N2 selectivity in 3% O2 at 200 °C. More importantly, it showed almost no activity loss in 200 ppm SO2 over a 15 h test. The theoretical calculations reveal that the negatively charged Pt has a stronger NO adsorption ability than the positively charged Pt, and Cu serves as the CO adsorption site. The much-weakened SO2 adsorption on Pt–CuO/CoAlO relative to the NO and CO adsorption effectively avoids the catalyst poisoning by SO2.
研究领域:
催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Chem
·
2019
·
IF 18.205
Rongan Shen,Wenxing Chen,Qing Peng,Siqi Lu,Lirong Zheng,Xing Cao,Yu Wang,Wei Zhu,Juntao Zhang,Zhongbin Zhuang,Chen Chen,Dingsheng Wang,Yadong Li
Summary The electrochemical direct synthesis of hydrogen peroxide (H 2 O 2 ) is significant but still challenging because of the lack of highly selective and active catalysts. Here, we report the synthesis of hollow nanospheres constructed by atomically dispersing platinum in amorphous CuS x support (h-Pt 1 -CuS x ) with a high concentration of single atomic Pt sites (24.8 at%), and this catalyst can consistently reduce O 2 into H 2 O 2 with selectivity of 92%–96% over a wide potential range of 0.05–0.7 V versus RHE in HClO 4 electrolyte. Scanning transmission electron microscopy and X-ray absorption fine structure spectroscopy confirmed the atomically isolated form of Pt with a low valance of +0.75. An electrochemical device that can synthesize H 2 O 2 directly from H 2 and O 2 is fabricated with H 2 O 2 productivity as high as 546 ± 30 mol kg cat − 1 h −1 . The well-defined and high-concentration single atomic Pt sites result in ultrahigh productivity of H 2 O 2 .
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Wen Yan,Jingxiang Sun,Tao Hu,Shuanghong Tian,Jinxi Feng,Ya Xiong
Single atom Pt was anchored on the surface of SiO 2 (Pt 1 /SiO 2 ) with the assistance of ionic liquid. It was found that Pt 1 (0.1 %)/SiO 2 could catalyze to sonically generate 3027.1 µmol L −1 h −1 H 2 O 2 , being 25.2 folds and 11.6 folds of those from pure ultrasound and sonocatalytic processes of Pt n (0.1 %)/SiO 2 , respectively. It was also the maximum concentration of H 2 O 2 generated by sonocatalysis so far. The significant boosting effect of Pt 1 was attributed to the synergetic role of its two-way catalytic processes proved by isotope labeling and DFT calculation. Firstly, Pt 1 catalyzed the sono-splitting of H 2 O to generate •OH as the precursor of H 2 O 2 formation by increasing the adsorption energy of H 2 O; Secondly, it catalyzed the combination of O 2 and •H to selectively generate •OOH as another precursor of H 2 O 2 by one end-on type adsorption of O 2 on Pt 1 . These findings provided a new way to enhance the ultrasonic generation of H 2 O 2 .
研究领域:
化学
·
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Shan Hu,Panzhe Qiao,Xinming Liang,Guiming Ba,Xiaolong Zu,Huilin Hu,Jinhua Ye,Defa Wang
Photoreduction of CO 2 and H 2 O into fuels and value-added chemicals is a promising green technology for solar-to-chemical conversion. However, improving the conversion efficiency with regulated product selectivity is a big challenge due to the sluggish dynamic transfer and insufficient active sites. Herein, we report on Pt single atoms anchored porous C 3 N 4 nanosheet photocatalyst (Pt 1 @CN) with Pt–N 4 coordination for stable and efficient CO 2 photoreduction using H 2 O as reductant. The Pt 1 @CN exhibits an evolution rate of 84.8 μmol g −1 h −1 with nearly 100% CO selectivity, outperforming most previous C 3 N 4 -based single-atom photocatalysts. Experimental and DFT calculation results reveal that the Pt–N 4 coordinated active sites promote the photogenerated electron transfer, CO 2 adsorption/activation, *COOH generation, and *CO desorption, thus accounting for the significantly improved CO 2 photoreduction activity with ∼100% CO selectivity. This study provides a deep insight into the significant roles of single-atom active sites in enhancing the CO 2 photoreduction activity and regulating the product selectivity.
研究领域:
材料科学
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环境科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-9
·
IF 15.7
Li Yan,Lu Lijun,Jiang Xueyu,Yang Dali,Chen Jeng-Lung,Dutta Chowdhury Abhishek,Li Wu,Pei Xianglin,Lei Aiwen
Biomass valorization is a way to promote the ‘waste-to-wealth’ concept, which is a pre-requisite condition for a future sustainable lifestyle. The direct utilization of natural polymer for value-added materials should be prioritized. With this object, we demonstrate a facile and economical method to prepare chitin-derived supramolecular nanowires-stabilized single-atom sites Pt catalysts (SS-Pt-CSNs). A comprehensive characterization shows the structure of single-atom Pt coordinated with the organic supramolecular (ligand-type) entity, which is both flexible (like in homogenous catalyst) and robust (like in heterogenous catalyst). Such hybrid characteristics of these SS-Pt-CSNs materials exhibit excellent catalytic performance for chemo-selective hydrogenation of various unsaturated bonds with a selectivity of more than 90:1 and a high turnover number (TON) of 121,350. Mechanistic studies demonstrate that both empty coordination sites of Pt and dynamic B-doping are the key factors for exceptional efficiency and high selectivity.
研究领域:
催化化学
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生物质转化
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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
Small
·
2023
·Vol. 19
·期 18
·2207240
·
IF 13.3
Yuanmeng Zhao,Yunhao Jiang,Yan Mo,Yueming Zhai,Juejing Liu,Andrew C. Strzelecki,Xiaofeng Guo,Changsheng Shan
It is critical to develop high-performance electrocatalyst for electrochemical nonenzymatic glucose sensing. In this work, a single-atom Pt supported on Cu@CuO core–shell nanowires (Pt 1 /Cu@CuO NWs) for electrochemical nonenzymatic glucose sensor is designed. Pt 1 /Cu@CuO NWs exhibit excellent electrocatalytic oxidation toward glucose with 70 mV lower onset potential (0.131 V) and 2.4 times higher response current than Cu NWs. Sensors fabricated using Pt 1 /Cu@CuO NWs also show high sensitivity (852.163 µA mM −1 cm −2 ), low detection limit (3.6 µM), wide linear range (0.01–5.18 µM), excellent selectivity, and great long-term stability. The outstanding sensing performance of Pt 1 /Cu@CuO NWs, investigated by experiments and density functional theory (DFT) calculations, is attributed to the synergistic effect between Pt single atoms and Cu@CuO core–shell nanowires that generates strong binding energy of glucose on the nanowires. The work provides a new pathway for exploring highly active SACs for electrochemical nonenzymatic glucose sensor.
研究领域:
电化学
·
催化
·
传感器
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）