JOURNAL OF CATALYSIS
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2026
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IF 6
Tingting Ge,Zhili Miao,Xiaorui Liu,Ziyan Jia,Chao Liu,Jiahui Huang
The oxidative esterification of alcohols is a key transformation in fine chemical synthesis and green chemistry. However, supported Au catalysts often suffer from nanoparticle agglomeration, leading to a significant loss of activity. Here, we report that Zn-doped hydroxyapatite (ZnHAP) can effectively stabilize ultra-small Au nanoclusters through Au-support interactions, even after high-temperature calcination at 400 ℃. The resulting Au/ZnHAP catalyst, with an ultralow Au loading of 0.25 wt%, exhibits outstanding performance in the base-free oxidative esterification of benzyl alcohol (Conv. 99%, Sele. 95%). Mechanistic investigations reveal that Zn incorporation into HAP modulates the surface basicity, thereby enhancing substrate adsorption and accelerating the key oxidative dehydrogenation step of the hemiacetal intermediate. Moreover, the increased Au 0 fraction induced by higher calcination temperatures further promotes benzyl alcohol activation. Consequently, under base-free conditions, the ester formation rate is governed by both the number of exposed Au active sites and the balanced distribution of surface acid–base sites. This work provides new mechanistic insights and practical guidance for the rational design of efficient, base-free oxidative esterification catalysts based on supported Au systems.
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ENERGY CONVERSION AND MANAGEMENT
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2016
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IF 4.801
Jian Huang,Yurong He,Li Wang,Yimin Huang,Baocheng Jiang
With water scarcity becoming an increasingly critical issue for modern society, solar seawater desalination represents a promising approach to mitigating water shortage. In addition, solar seawater desalination shows great potential for mitigating the energy crisis due to its high photo-thermal conversion efficiency. However, the increasing contamination of seawater makes it difficult to generate clean water through simple desalination processes. In this work, clean water is generated by a newly designed bifunctional Au@TiO 2 core-shell nanoparticle film with a high photo-thermal conversion efficiency that is capable of photocatalysis and solar evaporation for seawater desalination. Bifunctional films of Au@TiO 2 core-shell nanoparticles with good stability were prepared. It was found that the formation of the core-shell structures played a key role in promoting the photo-thermal conversion efficiency and the evaporation of seawater, while the photocatalytic function demonstrated herein could contribute to the purification of polluted seawater. Furthermore, the film structure can serve to concentrate the NPs for the photo-reaction, as well as heat for water evaporation, improving both the photo-reaction efficiency and photo-thermal conversion efficiency. This efficient approach to solar seawater desalination, which combines evaporation with the photodegradation of pollutants, could help to address the dual issues of water scarcity and water pollution.
研究领域:
材料科学
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环境工程
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纳米技术
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太阳能利用
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水净化
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SENSORS AND ACTUATORS B-CHEMICAL
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2022
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IF 9.221
Jinyu Huang,Jianwei Li,Zhonglei Zhang,Junda Li,Xiangdong Cao,Jihua Tang,Xuejin Li,Youfu Geng,Jiaqi Wang,Yu Du,Yatao Yang,Xiaofang Pan
Detecting trace ppb-level of formaldehyde (HCHO) in indoor ambient and human exhaled breath using metal oxide semiconductor (MOS) gas sensor has attracted increasing attention. Herein, Ag nanoparticles (Ag NP) modified In 2 O 3 and Au nanocage (Au NC) modified In 2 O 3 as well as bimetal Ag NP and Au NC co-modified In 2 O 3 were successfully prepared via one-step microwave-assisted solvothermal method and were used to construct semiconductor gas sensor. It is exciting to observe that the sensor based on Ag 6 Au 1 /In 2 O 3 exhibits the highest response of 277 toward 5 ppm HCHO at low operating temperature (170 °C), which is about 7 times, 38 times and 102 times higher than 6 wt. % Ag/In 2 O 3 , 1 wt. % Au/In 2 O 3 and pristine In 2 O 3 , respectively. Moreover, the selectivity and detection limit (down to 26 ppb) of Ag 6 Au 1 /In 2 O 3 sensor to HCHO have been proven to be greatly improved. This excellent sensing performance indicates that the proposed bimetal Ag and Au co-modification with synergistic catalysis effect offers an effective design for highly sensitive and efficient HCHO detection devices. Moreover, the mechanism of HCHO sensing with Au and Ag co-loaded In 2 O 3 was explored by the calculations obtained from first-principle density functional theory studies .
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COLLOIDS AND SURFACES B-BIOINTERFACES
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2023
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IF 5.8
Xinyu Cui,Minghui Li,Lei Tong,Miaojing Li,Xuefeng Tang,Xiaojun Han
Chemodynamic therapy (CDT) is based on the endogenous generation of cytotoxic hydroxyl free radicals (·OH) with high specificity and selectivity between cancer and normal cells. However, its efficacy is often limited by the relatively deficient catalytic activity of nanozymes in the tumor microenvironment (TME). Therefore, the combination of CDT with other strategy to realize synergistic therapy is necessary. Herein, a versatile plasmonic Au/Ag nanorods (abbreviated as Au/Ag NRs) via anisotropic Ag overgrowth on Au nanobipyramids was rationally devised to achieve synergistic nanozyme catalytic therapy and near infrared II (NIR-II) light induced photothermal therapy (PTT) with the guidance of computed tomography (CT) imaging. As TME contains high concentrations of H + and H 2 O 2 , Au/Ag NRs exhibited peroxidase (POD) activity to catalyze H 2 O 2 to produce ·OH, inducing cancer cell death. Meanwhile, Au/Ag NRs showed a preeminent NIR-II photothermal effect. More importantly, the enhanced ·OH generation by in-situ heating up resulting from PTT could conversely inhibit the expression of heat shock proteins (HSPs) to abate their resistance to PTT, realizing self-augmented synergistic effect. The NIR-II photothermally enhanced nanozyme catalytic cancer therapy validly inhibited the cancer proliferation, as demonstrated via both cell and animal assays. Moreover, ideal high-contrast CT imaging was realized, owing to the X-ray attenuation capability of elemental Au. The multifunctional Au/Ag NRs hold potential in oncotherapy with imaging capability, high efficiency and low side effects.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Yingying Li,Yanqiu Wang,Jing Lu,Wenwen Wang,Dong Wang
Smart windows are highly desired as emerging optical devices based on appealing sunlight modulation, however, some prevailing limitations remain with low photothermal conversion and narrow spectral adjusting ranges, which drastically restrict energy-saving performance. Herein, a strategically designed smart window achieves significant breakthroughs, containing photothermal fillers of Au nanoprisms (AuNPRs) hybrid MXene nanosheets, and copolymerized thermochromic poly( N -isopropyl acrylamide)-doped hyaluronic acid (HA) hydrogels. By harness of AuNPR@MXene nanocomposites as photo-trapped nanoheaters, stimulating thermo-responsive behaviors of hydrogels boosts solar transmittance switching. The compelling photothermal features depend on the amalgamation: thermoplasmonic effect of AuNPRs, broad-band-absorbed AuNPRs endowed by MXene, and thermal conductivity from AuNPRs to MXene, generating synergistic effects. We maximize the advancing transmittance regulation by controlling the proportion gain of HA to increase hydrogen-bonded interaction. The resulting device with low-loadings AuNPR@MXene composites (0.9 wt% and 0.98 vol%) is capable of allowing 78 % of the maximum visible light through before thermochromism and blocking 98.04 % of sunlight penetration when photothermal stimulation. Besides, outdoor measurements show an achievable great indoor temperature drop of about 7 °C only 30 min irradiation, and a skin-cooling performance in the wearable, illustrating the potential of adaptive solar modulation application.
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Biomaterials Science
·
2023
·Vol. 11
·期 4
·1335-1349
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IF 6.6
Hanchi Wang,Dongyang Wang,Huimin Huangfu,Siyu Chen,Qiuyue Qin,Sicong Ren,Yidi Zhang,Li Fu,Yanmin Zhou
Periodontitis is an inflammatory disease caused by bacterial infection. Excessive immune response and high levels of reactive oxygen species (ROS) further lead to the irreversible destruction of surrounding tissues. Developing new antimicrobial materials that regulate the immune system to resist inflammation can effectively treat periodontal inflammation. A nanoplatform integrating Ag+, photothermal therapy (PTT), and procyanidins (PC) for precision antibacterial and synergistic immunotherapy for periodontitis was proposed. This work loaded PC into AuAg nanoparticles, and the resulting nanocomposite was named AuAg-PC. PTT can effectively remove pathogenic bacteria, but high temperatures can cause tissue damage. Ag+ contributes to the preparation of a nanoparticle branched structure that improves the photothermal efficiency and helps PTT achieve an excellent antibacterial effect and avoid periodontal tissue damage. PC regulates host immunity by eliminating intracellular ROS, inhibiting inflammatory factors, and regulating macrophage polarisation in periodontal disease sites. It enhances the host's resistance to bacterial inflammation. AuAg-PC exerted an excellent anti-inflammatory effect and promoted tissue repair in animal periodontal inflammation models. Hence, AuAg-PC significantly combats periodontal pathogens and shows great application potential in the photothermal-assisted immunotherapy of periodontitis. This design provided a new controllable and efficient treatment platform for controlling persistent inflammation infection and regulating immunity.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Linjia Li,Rui Zhang,Yanhong Lin,Dejun Wang,Tengfeng Xie
The exploitation of morphological engineering strategies enables the design of semiconductor-based photocatalysts with a precision that significantly enhances their photocatalytic activity. In this study, a paradigm has been provided that embeds plasmonic nanostructures within the bulk of the semiconductor, which demonstrates an improvement in interfacial charge transfer and separation. It involves a distinct core-double shelled Au@carbon dots@CdS hybrid, exhibiting excellent photocatalytic H 2 generation under the visible light radiation. The interfacial engineering between the plasmonic nucleus and the semiconductor shell has been performed by the incorporation of carbon dots as faster charge channels. The effective driving force for plasmon-enhanced bulk charge separation of semiconductors and the unhindered interfacial charge transmission derived from carbon dots have been demonstrated by the use of steady state surface photovoltage (SPV) and transient state surface photovoltage (TPV) methods, as well as some intrinsic kinetics information of interfacial photoexcited charge carriers transfer processes.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
He Huang,Huahua Fan,Yuzhen Ge,Wanyue Ye,Yingcen Liu,Caicheng Song,Hua Lin,Xiaotong Zhang,Bing Li,Xiaowa Nie,Shufen Zhang,Rongwen Lu
The selective oxidation of the primary C H bonds in hydrocarbons to corresponding high-valued oxygenates is highly desired but challenging to realize. The difficulty arises from the high homolytic bond dissociation enthalpy of the C H bond, the relatively high reactivity of oxygenated intermediates, and the diversity of resultant products. Herein, we reported the in situ confinement of Au clusters in Silicalite-1 for the selective solvent-free oxidation of toluene to benzaldehyde. The doping of an alkali metal (K or Na) resulted in the formation of electron-rich Au species, which readily facilitate the activation of oxygen, In turn, toluene is activated by the produced reactive oxygen species in a single step, as confirmed through density functional theory (DFT) calculations. At optimal alkali metal doping, the selectivity to benzaldehyde could reach > 90 %, with the toluene conversion being 19.8 %. Remarkably, the total turnover number (TTN) of Au@Silicalite-1–0.2 K was found to be 29,658, which is one or two orders of magnitudes higher than the previously reported values. These findings are expected to inspire the design of highly efficient catalysts for the activation of fundamental feedstock with C H bonds.
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ANALYTICA CHIMICA ACTA
·
2022
·
IF 6.911
Hongying Li,Jiale Zhang,Lingling Jiang,Ruo Yuan,Xia Yang
The identification of enantiomers is of great importance in chiral separations and medicinal chemistry . While Surface-enhanced Raman spectroscopy (SERS) is a technique that provides vibrational fingerprints of analytes . The enantiomers identification relies on the SERS difference between left and right-handed circularly polarized light or additional selectors for indirect distinction. In this work, Au–Ag core shell nanobipyramid (L/ [email protected] BPs) were synthesized guiding by chiral encoder of L/D-cysteine. L/ [email protected] BPs produced plasmon-induced circular dichroism signals in the plasmon resonance absorption band , which can be tuned by modulation the amount of cysteine. Moreover, the chiral anisotropy factor of L/ [email protected] BPs at 532 nm can reach 5.11 × 10 −3 . Due to the selective resonance coupling between L/ [email protected] BPs and different enantiomers, L/ [email protected] BPs were further used as SERS substrates for efficient discrimination of biologically relevant small molecules . Chiral [email protected] BPs display the potential for chiral drug identification.
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RARE METALS
·
2022
·Vol. 42
·期 4
·1274-1282
·
IF 6.318
Zha Ai-Yun,Zha Qing-Bing,Li Zhi,Zhang Hong-Min,Ma Xue-Feng,Xie Wen,Zhu Ming-Shan
Bisphenol A (BPA), one of the most commonly used plastic organic monomers, is widely used in manufacturing food packaging and containers. However, the gradual emissions of BPA from manufacturing plastic products bring great potential in human health threats, which urgently need to develop a simple and rapid method for detecting BPA. Cetyltrimethylammonium bromide (CTAB), a typical surfactant, is used to enhance the electrochemical detection of trace endocrine disruptors due to the fact that it can effectively enrich and absorb hydrophobic phenolic compounds through the hydrophobicity of its long-chain alkanes. Based on these, the present study reports a ternary composite of Au on zinc oxide/reduced graphene oxide nanosheets (Au/ZnO/rGO) as electrochemical sensor for detecting BPA. With the addition of CTAB, the analytic performances toward BPA detection are significantly improved 3.8 times compared with those without CTAB. The pH, accumulation potential and time are optimized. Moreover, the electrochemical activity of CTAB/Au/ZnO/rGO sensor is also evaluated by cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), differential pulse voltammetry (DPV) and scan rate. The sensor displays two linear range from 10 to 1340 nmol·L −1 and 1340 to 10,000 nmol·L −1 , and a low detection limit of 4.95 nmol·L −1 . Lastly, the sensor also exhibits good reproducibility, selectivity and potential practical application for BPA detection in real samples. Graphical abstract
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SENSORS AND ACTUATORS B-CHEMICAL
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2022
·
IF 9.221
Long Chen,Haozhou Shi,Chenjia Ye,Xiaoyu Xia,Yi Li,Chenying Pan,Yanhua Song,Jun Liu,Hao Dong,Di Wang,Xing Chen
In this work, Au decorated In-doped SnO 2 (Au@In 2 O 3 -SnO 2 ) porous nanotubes (PNTs) were fabricated via electrospinning and a subsequent calcination treatment. The In-doped SnO 2 PNTs with various Au/Sn molar ratios possessed good ethanol sensing properties. As a result, the 3 % mol Au decorated In-doped SnO 2 PNTs had high response to ethanol (R a /R g = 316.8–100 ppm) and can detect ethanol down to 50 ppb at a low working temperature of 150 °C. In addition, the gas sensor also had high selectivity, good reversibility and long-term stability. The enhanced sensing performance was mainly ascribed to the increase of oxygen vacancies , catalytic activity of Au nanocatalysts, and porous structures . The sensing results demonstrated that Au@In 2 O 3 -SnO 2 PNTs had the great potential for ethanol detecting, and provide a facile method for rationally designing other types of gas sensors.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Muhammad Humayun,Habib Ullah,Zhuo-Er Cheng,Asif Ali Tahir,Wei Luo,Chundong Wang
Highly efficient photocatalytic water reduction to evolve hydrogen can be achieved by the construction of Z-scheme systems that mimics natural photosynthesis. However, coupling appropriate semiconductors with suitable water reduction potential still remains challenging. Herein, we report a novel Z-scheme system, based on the Au decorated 5,10,15,20-tetrakis(4-trimethylammoniophenyl) porphyrin tetra(p-toluene sulfonate) functionalized iron-doped carbon nitride . We prepared carbon nitride by varying the amount of iron dopant and then functionalized with porphyrin to obtain heterostructure photocatalyst. Owing to the strong interfacial contact and proper band alignment, a Z-scheme system is fabricated. Finally, we deposited Au nanoparticles over the surface of the as-fabricated Z-scheme system to promote the surface redox properties via efficient charge carrier’s separation and transfer. The 3Au-3 P/30Fe-CN photocatalyst achieved excellent H 2 evolution activity by producing 3172.20 µmol h −1 g −1 under UV–visible irradiation. The calculated quantum efficiencies for 3Au-3 P/30Fe-CN photocatalyst at 365 and 420 nm irradiation wavelengths are 7.2% and 3.26%, respectively. The experimentally observed efficiency of our photocatalyst is supported by the density functional theory simulations in terms of the lowest work function and strong electrostatic interaction among the constituents of Z-scheme system.
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