ACS Catalysis
·
2025
·
IF 13.1
Lingfang Liu,Liangyan Deng,Yachao Wang,Yu Wang,Yaxiong Wei,Guofeng Zhao,Cong Fu
Photocatalytic oxidative coupling of methane (OCM) represents a promising route for chemical and fuel synthesis, yet the development of photocatalysts with high activity and selectivity remains challenging. Here, we demonstrate a synergistic ensemble of Au nanoparticles and Li-doped TiO2 that significantly enhances photocatalytic OCM performance in a flow reactor. The optimized catalyst achieved a C2 hydrocarbon production rate of 4.1 mmol g–1 h–1 with selectivity up to 97% and maintained robust stability over 50 h. Comprehensive mechanistic studies, employing in situ transient absorption spectroscopy (TAS), in situ electron paramagnetic resonance (EPR), and operando diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) techniques, indicate that Li dopants facilitate the formation of bulk/surface defects by a unique bulk-to-surface-to-gas Li migration process. These induced defects serve a dual role: bulk defects act as effective hole traps, while surface defects provide active sites that enhance charge transfer and promote O2 adsorption/activation. Combined with Au acting as a methane activation center, this synergy promotes efficient C–H activation and C–C coupling, thus contributing to its superior catalytic performance. This work provides critical mechanistic insights into photocatalytic OCM and underscores the potential of surface and bulk engineering for efficient photocatalytic processes.
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高影响因子
FOOD RESEARCH INTERNATIONAL
·
2021
·
IF 6.475
Mengke Zhang,Mengyin Li,Yan Zhao,Naifeng Xu,Lanlan Peng,Yuanfeng Wang,Xinlin Wei
In this study, a rapid sandwich immunochromatographic assay (ICA) was developed to detect parvalbumin (PV). Firstly, two optimum primary monoclonal antibody (mAb) against PV had been screened out: mAb1 was used as the capture antibody, and mAb2 conjugated to Fe 3 O 4 /Au nanoparticles (Fe 3 O 4 /AuNPs) that served as a detection reagent. Using this pair of mAbs, a sandwich ICA strip based on Fe 3 O 4 /AuNPs was developed. The results showed that the color intensity of test line positively correlated with the PV concentration in the standard or spiked sample. The limit of detection for qualitative (LOD) and quantitative detection (LOQ) were 2 ng/mL and 0.691 ng/mL, respectively. Besides, the detection time of this ICA strip was within 15 min. The recovery rates ranged from 104.0% to 117.4%, within an acceptable level (80–120%). Moreover, the developed assay also showed high cross reaction in different fish species. These results demonstrated that the established test strip has the potential to be used as a rapid screening tool for large scale determination of PV in foodstuffs.
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PubMed
高影响因子
Nanomedicine-Nanotechnology Biology and Medicine
·
2015
·
IF 6.155
Jinrui Gan,Xiang Wei,Yixin Li,Jiao Wu,Kun Qian,Baohong Liu
We report a novel platform using optimized SiO 2 @Au core–shell structures as matrices for highly efficient laser desorption/ionization mass spectrometry analysis of small biomolecules (MW < 700 Da). Owing to the designer structure, SiO 2 @Au nanoshells can achieve low detection-of-limits (~ pmol–fmol) in mass spectrometry and selective laser desorption/ionization in bio-mixtures towards diverse small molecules. By further surface modification with aptamers , Apt-SiO 2 @Au nanoshells allowed simultaneously targeted enrichment and detection of kanamycin with a detection limit at 200 pM. Our work not only starts new applications of SiO 2 @Au nanoshells in mass spectrometry, but also contributes to advanced analysis of either a group of small molecules or one target small molecule from complex bio-samples in a pre-designed manner for bio-diagnostics. From the Clinical Editor Existing methods for the detection of small molecules are often not sensitive enough. Here, the authors developed aptamer functionalized [email protected] nanoshells for use in mass spectrometry, with very low detection limits. The new platform appeared to be simple and efficient and should be applicable in detection of clinical samples.
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Small
·
2024
·Vol. 20
·期 32
·2311840
·
IF 13
Xinhua Zhao,Lingling Du,Xiaxia Xing,Zhenxu Li,Yingying Tian,Xiaoyu Chen,Xiaoyan Lang,Huigang Liu,Dachi Yang
With the recently-booming hydrogen (H 2 ) economy by green H 2 as the energy carriers and the newly-emerged exhaled diagnosis by human organ-metabolized H 2 as a biomarker, H 2 sensing is simultaneously required with fast response, low detection limit, and tolerant stability against humidity, switching, and poisoning. Here, reliable H 2 sensing has been developed by utilizing indium oxide nanocubes decorated with palladium and gold nanodots (Pd–Au NDs/In 2 O 3 NCBs), which have been synthesized by combined hydrothermal reaction, annealing, and chemical bath deposition. As-prepared Pd–Au NDs/In 2 O 3 NCBs are observed with surface-enriched NDs and nanopores. Beneficially, Pd–Au NDs/In 2 O 3 NCBs show 300 ppb-low detection limit, 5 s-fast response to 500 ppm H 2 , 75%RH-high humidity tolerance, and 56 days-long stability at 280 °C. Further, Pd–Au NDs/In 2 O 3 NCBs show excellent stability against switching sensing response, and are tolerant to H 2 S poisoning even being exposed to 10 ppm H 2 S at 280 °C. Such excellent H 2 sensing may be attributed to the synergistic effect of the boosted Pd–Au NDs’ spillover effect and interfacial electron transfer, increased adsorption sites over the porous NCBs’ surface, and utilized Pd NDs’ affinity with H 2 and H 2 S. Practically, Pd–Au NDs/In 2 O 3 NCBs are integrated into the H 2 sensing device, which can reliably communicate with a smartphone.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xuan Huang,Ming Yi,Kewen Tang
To address resources shortage and environmental degradation, noble metal recovery from e-waste is in desperate need. Herein, to achieve selective extraction of gold (Au) and palladium (Pd) from practical e-waste, a series of tridentate thioether extractants are designed with ester functional groups at both ends of the thioether. By varying the chain length of the ester alkyl, the relationship between extractant structure and performance is further explored. The results indicate that the as-introduced tridentate structure facilitate the Au(III) and Pd(II) extraction, demonstrating a complex mechanism involving both coordination substitution and ion association. Notably, the extractant with the shortest carbon chain length and smallest molecular weight delivers outstanding extraction capacities of 920.2 mg/g for Au(III) and 280.7 mg/g for Pd(II). More importantly, it exhibits superior selectivity (∼100 %) for Au(III) and Pd(II) in complex metal solutions. This work guides the design of thioether-based extractants for sustainable recovery of noble metal from practical e-waste.
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高影响因子
ANALYTICA CHIMICA ACTA
·
2023
·
IF 6.2
Kai-Xin Xie,Rui-Ping Huo,Xiu-Li Song,Qiao-Ling Liu,Yue Jiang,Yu-Han Li,Lu-Lu Dong,Jia-Xin Cheng
Surface plasmon coupled emission (SPCE), a novel surface-enhanced fluorescence technique, can generate directional and amplified radiation by the intense interaction between fluorophores and surface plasmons (SPs) of metallic nanofilms . For plasmon-based optical systems, the strong interaction between localized and propagating SPs and “hot spot” structures show great potential to significantly improve the electromagnetic (EM) field and modulate optical properties . Au nanobipyramids (NBPs) with two sharp apexes to enhance and restrict the EM field were introduced through electrostatic adsorption to achieve a mediated fluorescence system, and the emission signal enhancement was realized by factors over 60 compared with the normal SPCE. It has been demonstrated that the intense EM field produced by the NBPs assembly is what triggered the unique enhancement of SPCE by Au NBPs, which effectively overcomes the inherent signal quenching of SPCE for ultrathin sample detection. This remarkable enhanced strategy offers the chance to improve the detection sensitivity for plasmon-based biosensing and detection systems, and expand the range of applications for SPCE in bioimaging with more comprehensive and detailed information acquisition. The enhancement efficiency for various emission wavelengths was investigated in light of the wavelength resolution of SPCE, and it was discovered that enhanced emission for multi-wavelength could be successfully detected through the different emission angles due to the angular displacement caused by wavelength change. Benefit from this, the Au NBP modulated SPCE system was employed for multi-wavelength simultaneous enhancement detection under a single collection angle, which could broaden the application of SPCE in simultaneous sensing and imaging for multi-analytes, and expected to be used for high throughput detection of multi-component analysis.
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TALANTA
·
2021
·
IF 6.057
Shemsu Ligani Fereja,Ping Li,Jinhan Guo,Zhongying Fang,Ziwei Zhang,Zhihua Zhuang,Xiaohui Zhang,Kaifan Liu,Wei Chen
Folic acid (FA) is the natural form of water-soluble vitamins widely found in most plants and animal products and its deficiency leads to several human body abnormalities. The advancements of metal nanoclusters are highly increasing due to their molecule-like optical properties and attractive applications. Because of increasingly demand of noble metal nanoclusters as sensing templates, different synthesis methods have been developed for facile synthesis of noble metal nanoclusters . Herein, red-emitting fluorescent bovine serum albumin (BSA)-capped Au–Ag bimetallic NCs are facilely synthesized through green one-pot synthetic approach. The effect of silver on the fluorescence properties of Au NCs was investigated and it was found that introduction of silver can enhance the fluorescence intensity . The fluorescence intensity of the as-prepared Au–Ag nanoclusters gets quenched in the presence of folic acid in an aqueous medium and it was used as ultrasensitive sensing probe for FA detection. The developed Au–Ag NCs-based sensing probe shows linear response in the wide range of 0–100 μM and the detection limit is as low as 0.47 nM. Its applicability has also been confirmed successfully in real human serum, urine and FA tablet samples. Due to the high stability, sensitivity and selectivity , the developed bimetallic cluster sensing system is highly promising to be applied in the pharmaceutical and clinical laboratories.
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Small
·
2020
·Vol. 17
·期 27
·1907114
·
IF 11.459
Qinzhen Li,Jinsong Chai,Sha Yang,Yongbo Song,Tao Chen,Cheng Chen,Hui Zhang,Haizhu Yu,Manzhou Zhu
Thiolate-protected nanoclusters with different charge states usually show similar structure frameworks but different electronic configurations, which are proved to dramatically affect their properties such as magnetism, photoluminescence, and catalytic activity. Until now, few nanoclusters with alterable charge states have been reported and only some of them are structurally solved, limiting the in-depth studies on their interesting properties. Here, a new Au Cu alloy nanocluster [Au 18 Cu 32 (SPhCl) 36 ] 2− (HSPhCl = 4-chlorophenylthiophenol) is synthesized and structurally solved by X-ray crystallography. Interestingly, it is found that this nanocluster can be reduced to another nanocluster with a different charge state, that is, [Au 18 Cu 32 (SPhCl) 36 ] 3− . This change in charge states is clearly proved by X-ray crystallography, electrospray ionization mass spectrometry, thermogravimetric analysis, and electron paramagnetic resonance. Furthermore, several redox methods are carried out to realize the reversible interconversion between these two nanoclusters, including electrochemical redox, introduction of H 2 O 2 /NaBH 4 , and oxidation with silica under air atmosphere. This work offers new insight into the transform progress of charge states with Au Cu alloy nanoclusters which contributes to the understanding of the relationship between electronic structure and properties of nanoclusters and further development of Au Cu nanoclusters with excellent performance.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-7
·
IF 16.6
Li Peihui,Hou Songjun,Wu Qingqing,Chen Yijian,Wang Boyu,Ren Haiyang,Wang Jinying,Zhai Zhaoyi,Yu Zhongbo,Lambert Colin J.,Jia Chuancheng,Guo Xuefeng
The transformation from one compound to another involves the breaking and formation of chemical bonds at the single-bond level, especially during catalytic reactions that are of great significance in broad fields such as energy conversion, environmental science, life science and chemical synthesis. The study of the reaction process at the single-bond limit is the key to understanding the catalytic reaction mechanism and further rationally designing catalysts. Here, we develop a method to monitor the catalytic process from the perspective of the single-bond energy using high-resolution scanning tunneling microscopy single-molecule junctions. Experimental and theoretical studies consistently reveal that the attack of a halogen atom on an Au atom can reduce the breaking energy of Au−S bonds, thereby accelerating the bond cleavage reaction and shortening the plateau length during the single-molecule junction breaking. Furthermore, the distinction in catalytic activity between different halogen atoms can be compared as well. This study establishes the intrinsic relationship among the reaction activation energy, the chemical bond breaking energy and the single-molecule junction breaking process, strengthening our mastery of catalytic reactions towards precise chemistry.
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高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2020
·
IF 6.155
Kaili Yao,Xiaojun Tan,Bing Dai,Jie Bai,Qiaoyang Sun,Wenxin Cao,Jiwen Zhao,Lei Yang,Jiecai Han,Jiaqi Zhu
Boron doped diamond (BDD) electrode is a promising electrochemical material for detecting dopamine level in the human’s body. In this work, we developed a new doping source - graphite and solid boron oxide powders to synthesize BDD film with microwave plasma chemical vapor deposition , so as to avoid using toxic or corrosive dopants , such as boroethane and trimethylborate. The synthesized BDD film is pinhole free and with high doping density of 8.44 × 10 20 cm −3 calculated from the Raman spectroscopy . Subsequently, Au nanospheres were decorated on the surface of BDD film to improve electrochemical performance of the BDD film. The Au nanoparticles modified BDD electrode demonstrates an excellent electrochemical response, a high sensitivity (in the range of 5 μM-1 mM), and a low detection limit (∼ 0.8 μM) for detecting dopamine.
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高影响因子
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2024
·Vol. 416
·期 19
·4417-4426
·
IF 3.8
Zhu Zhentong,Wang Xiaoli,Wang Na,Zeng Chaoqin,Zhang Lei,Fan Jiamin,Yang Xin,Li Peizhe,Yuan Hongxia,Feng Yanjun,Huo Shuhui,Lu Xiaoquan
Artificial enzymes with high stability, adjustable catalytic activity, controllable preparation, and good reproducibility have been widely studied. Noble metal nanozymes, particularly gold nanoparticles (Au NPs), exhibit good catalytic activity, but their stability is poor. In this study, zeolitic imidazolate framework-8 (ZIF-8) was used as a carrier for Au NPs, thus improving the utilization efficiency and conservation stability of the nanozymes. A ZIF-8/Au nanocomposite with peroxidase activity and a raspberry-shaped structure was synthesized. In the assay, ZIF-8/Au catalyzed the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to a blue product oxidized TMB (oxTMB). Glutathione (GSH) selectively inhibited this reaction, with a detection limit of 0.28 µM and linear range of 0.5–60 µM. Using the photo and chromaticity analysis functions, we developed a portable analysis method using a smartphone equipped with a camera module as a detection terminal for a wide range of rapid screening techniques for GSH. Preparation of raspberry-shaped ZIF-8/Au improved the catalytic activity of Au NPs and good results were demonstrated in serum, which suggests their promising application under physiological conditions. Graphical Abstract
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高影响因子
Catalysts
·
2020
·Vol. 10
·期 11
·1285
·
IF 3.52
Hao Gan,Wenzhao Han,Jiadi Liu,Juntian Qi,Hui Li,Liping Wang
Being superior to natural enzymes, nanoenzymes are drawing a great deal of attention in the field of biosensing. Herein, we developed an ultrasensitive, stable and selective colorimetric assay having dual functionalities of Au-tipped Pt nanorods (NRs). The optical and catalytic properties of Au-tipped Pt NRs were monitored using a spectrophotometer and the chromogenic substrate 3, 3′, 5, 5′-tetramethylbenzidine (TMB) in the presence of H2O2, respectively. We found that Au-tipped Pt NRs exhibited excellent peroxidase-like activity, which decomposed hydrogen peroxide (H2O2) into oxygen (O2). The produced O2oxidized the chromogenic substrate into a blue color product. The oxidation rate of the chromogenic substrate could be monitored using a spectrophotometer at 652 nm. Notably, the peroxidase-like activity of Au-tipped Pt NRs decreased in the presence of ascorbic acid (AA). The produced O2preferentially reacted with AA, generating ascorbyl radicals (AA·) instead of oxidizing TMB, and thereby decreased the oxidation rate of TMB. Based on this inhibitory property, a selective colorimetric assay was developed using Au-tipped Pt NRs for the detection of AA. This work offers a novel detection method for AA.
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