Chemical Science
·
2026
·
IF 7.4
Yue Feng,Yu-Qi Wang,Jiaju Fu,Zi-Cong Wang,Dong Wang,Li-jun Wan
Understanding the in situ surface structure of electrodes is crucial for unraveling the synergistic mechanisms of electrolytes in interfacial electrocatalysis. Herein, using in situ electrochemical scanning tunneling microscopy (EC-STM), we unveil the electrolyte concentration-driven roughening of Au(111) surfaces under cathodic polarization. As the concentration of alkali metal cations (AM+) ([AM+]) decreases, the AM+-induced surface structure evolution proceeds from surface corrosion at 1 M, to the formation of surface pits alongside surface nanoclusters composed of released Au atoms at 0.5-0.3 M, and ultimately to the generation of pit-free nanoclusters via surface atomic migration at 0.2 M. Moreover, surface modifications modulate the electrode surface structure, enabling more pronounced structure evolution at lower bulk [AM+]. Electrochemical measurements correlate increased surface roughness with enhanced CO2 reduction reaction (CO2RR) performance. The results provide new perspective on understanding the role of AM+ in regulating the electrochemical interface, and microscopic insights into AM+ concentration-driven in situ surface structures, which is important for understanding electrolyte-mediated surface structure-activity relationships.
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ENVIRONMENTAL GEOCHEMISTRY AND HEALTH
·
2026
·Vol. 48
·期 12
·509
·
IF 4.3
Abudureyimu Mukaidasi,Chen Xi,Zhu Xiaoxuan,Huang Yu,Wang Yehui
Naphthalene, as a representative polycyclic aromatic hydrocarbon (PAH), is persistent, bioaccumulative, and toxic, posing a long-term threat to aquatic environments. To address this issue, a mineral-mediated Au-TiO 2 /g-C 3 N 4 composite photocatalyst with coupled adsorption and photocatalytic functions was constructed through photodeposition, co-pyrolysis, and subsequent in situ mineral loading/calcination. Characterization analyses demonstrated that 1.0 wt% Au provided the most effective electronic modulation, giving an apparent rate constant of 0.174 min −1 for naphthalene degradation, which was 3.78 times that of the Au-free counterpart. Among the tested mineral supports, bentonite exhibited the strongest adsorption-enrichment effect, increasing the adsorption efficiency to 47.2% and enabling complete removal and near-complete mineralization of naphthalene within 25 min of irradiation. Radical trapping experiments and ESR spectra identified ·OH, ·O 2 − , and h + as the dominant reactive species. Combined with Gas Chromatography-Mass Spectrometry (GC-MS) and in situ Gas Chromatography (GC) analyses, naphthalene was found to undergo progressive hydroxylation, ring opening, and oxidation before final mineralization. This work provides a feasible strategy for designing mineral-semiconductor composite photocatalysts for efficient PAH removal from water.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Xu Yueshan,Wu Daoxiong,Zhang Qinghua,Rao Peng,Deng Peilin,Tang Mangen,Li Jing,Hua Yingjie,Wang Chongtai,Zhong Shengkui,Jia Chunman,Liu Zhongxin,Shen Yijun,Gu Lin,Tian Xinlong,Liu Quanbing
The direct oxidation of methane to methanol under mild conditions is challenging owing to its inadequate activity and low selectivity. A key objective is improving the selective oxidation of the first carbon-hydrogen bond of methane, while inhibiting the oxidation of the remaining carbon-hydrogen bonds to ensure high yield and selectivity of methanol. Here we design ultrathin Pd x Au y nanosheets and revealed a volcano-type relationship between the binding strength of hydroxyl radical on the catalyst surface and catalytic performance using experimental and density functional theory results. Our investigations indicate a trade-off relationship between the reaction-triggering and reaction-conversion steps in the reaction process. The optimized Pd 3 Au 1 nanosheets exhibits a methanol production rate of 147.8 millimoles per gram of Pd per hour, with a selectivity of 98% at 70 °C, representing one of the most efficient catalysts for the direct oxidation of methane to methanol.
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Analytical Methods
·
2014
·Vol. 6
·期 17
·6789-6795
·
IF 1.938
Wei Li,Zhao Gao,Rongxin Su,Wei Qi,Libing Wang,Zhimin He
Pepsin is an active digestive enzyme present in the acidic environment of animal stomachs, and has been widely used to prepare bioactive peptides in the food industry. In this work, a simple fluorescence sensor for scissor-based detection of pepsin activity was developed by using lysozyme-stabilized gold nanoclusters (AuNCs@Lyz) in aqueous media. Under acidic conditions (pH 3.0), enzymatic digestion of AuNCs@Lyz with pepsin results in a significant decrease of fluorescence intensity. Notably, its acidic environment not only helps maintain the maximum fluorescence of gold nanoclusters, but also ensures the highest enzymatic activity of pepsin. In addition to offering high selectivity because of the unique proteolytic action of pepsin under acidic conditions, this facile method provides high sensitivity. With the sensing system, the linear range for pepsin detection is found to be 1 μg mL−1 to 100 μg mL−1, with a detection limit of 0.256 μg mL−1 at a signal-to-noise ratio of 3. Furthermore, the AuNCs@Lyz based fluorescent sensing system could find applications in highly sensitive and selective detection of pepsin in food and biological samples.
研究领域:
生物化学
·
食品科学
·
分析化学
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Energy Sources Part A-Recovery Utilization and Environmental Effects
·
2019
·
IF 0.894
Qian Du,Junjie Xu,Zhiyang Cheng,Jianmin Gao
Research on the application of nano-fluids into the direct absorption solar collector represents a prospective approach to solving the problem of high thermal losses of traditional solar collection systems. In this work, Au, CuS and Au-CuS blended Nanoparticles (NPs) were synthesized and the solar photo-thermal conversion performance of them was studied in an experimental investigation. According to the analysis of the results of the experiment, we knew that the temperature and photo-thermal conversion efficiency rised markedly as the light intensity and concentration increase. Our work found that mixing different NPs to match the solar spectral intensity can prepare working fluids for solar photo-thermal conversion instead of increasing the volume fraction of the same NP. When the concentration ratio of Au-CuS blended nanoparticles is 4:6, the conversion efficiency is the highest, reaching 26.04%.
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JOURNAL OF MODERN OPTICS
·
2014
·
IF 1.166
Cheng Qian,Enze Xu,Ning Sui,Yinghui Wang,Honglin Wu,Yunfei Song,Zhihui Kang,Hanzhuang Zhang
The photoluminescence (PL) characteristics of MEH-PPV hybrid films blended with Au nanoparticles are studied in detail. Due to the strong coupling effect between the surface plasmon of Au nanoparticles and the emission of MEH-PPV, the introduction of Au nanoparticles could enhance the PL intensity and modulate the shape of absorption and excitation spectra, according to our steady spectroscopy experiments. Besides, the relaxation dynamic experiments show that the non-radiative rate in the hybrid system decreases. The temperature and the excitation intensity (EI)-dependent PL spectral data indicate that hybrid MEH-PPV films have lower activation energy and higher thermal exchange rate. As a result, the thermal accumulation effect and the non-linearity of EI-induced PL enhancement are suppressed in hybrid films.
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INTERNATIONAL JOURNAL OF HEAT AND MASS TRANSFER
·
2017
·
IF 3.458
Meijie Chen,Yurong He,Jiaqi Zhu
In this study, the solar photothermal conversion performance of bimetallic Au–Ag nanoparticles (NPs) was investigated experimentally. NPs were prepared using a sodium citrate thermal reduction method, using the same procedure and materials to maintain the same particle surface properties. NPs with a tunable plasmon resonance wavelength and demonstrating a high intensity in the visible region were obtained by adjusting the molar ratio of Ag to Au precursors. Experimental results show that blended Au–Ag NPs exhibit a solar photothermal conversion efficiency of 31.41%, which lies between the values of pure Au and Ag NPs under the same NP volume fraction due to the independently scatter light of the Au and Ag NPs in this composite system. Bimetallic Au–Ag NPs demonstrated the highest solar photothermal conversion efficiency of 41.37%, a 31.7% increase over that of blended Au–Ag NPs. The efficiency of the bimetallic Au–Ag NP system was also higher than that of the pure Au NPs (37.81%) with a 40% decrease in Au consumption.
研究领域:
纳米材料
·
太阳能转换
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等离激元学
·
光热材料
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Haiyan Kang,Yulong Luo,Chaopeng Liu,Zhongxian Song,Chaohai Wang,Xu Yan,Mengxia Ma,Xiaole Yan,Deming Gu,Yanli Mao
The recovery of Au(III) by adsorption has attracted extensive attention since it promotes solving the problems of environmental pollution and resource waste. Herein, we prepared the functionalized MCM-41 (MCM-NH 2 -OH) and explored the synergistic adsorption effects for Au(III). The adsorption capacity of MCM-NH 2 -OH reached 1664.9 mg·g −1 , which was 15.98 times and 2.99 times higher than MCM-NH 2 (104.2 mg·g −1 ) and MCM-OH (556.0 mg·g −1 ), respectively. The fitting kinetics experiments demonstrated that Au(III) adsorption by MCM-NH 2 -OH was conformed to the pseudo-second-order kinetic model. The adsorption rate of MCM-NH 2 -OH (2.62 × 10 -2 g·mg −1 ·min −1 ) was 346.1 times higher than MCM-NH 2 (7.57 × 10 -5 g·mg −1 ·min −1 ). The adsorption mechanism and the role of –NH 2 and –OH groups were investigated by XPS, XRD, and FTIR. More Au(III) can be adsorbed on –NH 2 groups by electrostatic attraction and chelation that provided electron acceptor for –OH groups, which further enhanced the reduction of Au(III) to Au(0). Further, MCM-NH 2 -OH exhibited superior selectivity and reusability for Au(III). Therefore, the synergy between –NH 2 and –OH groups is suitable for efficient adsorption-recover of gold applied in actual wastewater.
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CARBOHYDRATE POLYMERS
·
2022
·
IF 10.723
Lingyuan Chen,Jiali Tang,Suoque Wu,Shixing Wang,Zhaogang Ren
A pyridine-modified chitosan ( PMCS ) adsorbent with excellent adsorption performance and specific selectivity for Au(III) in wastewater was prepared. FTIR, SEM, XPS and XRD were used to study its adsorption performance, and various models were used to fit and analyze the experimental adsorption data. The maximum adsorption capacity of PMCS for Au(III) is 549.41 mg/g (298 K, pH = 4). The data analysis results prove that the PSO and Langmuir models best describe the adsorption process. Adsorption experiments in the presence of multiple ions proved that PMCS is selective for the adsorption of Au(III). The adsorption and desorption experiments showed that the adsorption rate of PMCS could still reach 94.77% after three cycles. In summary, PMCS was demonstrated to be a high-quality material for the adsorption of Au(III) from wastewater due to its excellent adsorption performance, specific selectivity and reusability.
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RSC Advances
·
2022
·Vol. 12
·期 10
·6205-6213
·
IF 4.036
Chao Cai,Shaobo Han,Xiaotao Zhang,Jingxia Yu,Xia Xiang,Jack Yang,Liang Qiao,Xiaotao Zu,Yuanzheng Chen,Sean Li
Oxygen evolution reaction (OER) has attracted enormous interest as a key process for water electrolysis over the past years. The advance of this process relies on an effective catalyst. Herein, we employed single-atom Au doped Co-based nanosheets (NSs) to theoretically and experimentally evaluate the OER activity and also the interaction between Co and Au. We reveal that Au–Co(OH)2 NSs achieved a low overpotential of 0.26 V at 10 mA cm−2. This extraordinary phenomenon presents an overall superior performance greater than state-of-the-art Co-based catalysts in a sequence of α-Co(OH)2 < Co3O4 < CoOOH < Au–Co(OH)2. With ab initio calculations and analysis in the specific Au–Co(OH)2 configuration, we reveal that OER on highly active Au–Co(OH)2 originates from lattice oxygen, which is different from the conventional adsorbate evolution scheme. Explicitly, the configuration of Au–Co(OH)2 gives rise to oxygen non-bonding (ONB) states and oxygen holes, allowing direct O–O bond formation by a couple of oxidized oxygen with oxygen holes, offering a high OER activity. This study provides new insights for elucidating the origins of activity and synthesizing efficient OER electrocatalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Yueshan Xu,Daoxiong Wu,Peilin Deng,Jing Li,Junming Luo,Qi Chen,Wei Huang,Chong Michael Shim,Chunman Jia,Zhongxin Liu,Yijun Shen,Xinlong Tian
The direct methane (CH 4 ) oxidation to high value-added C1 chemicals is a great promising strategy to explore the CH 4 resource utilization. However, the low activity and selectivity of catalytic performance remains a great conundrum due to the difficulty to activate the C H bond and the unmanageable over oxidation. Herein, Pd x Au y nanowires (NWs) with various Pd/Au atomic ratios are presented as ideal models to explore the atomic-level effect of PdAu atoms for the direct CH 4 oxidation. The influence of reaction parameters are systematically investigated, and Pd 9 Au 1 NWs display a maximum yield of 2890.3 μmol g −1 h −1 with 99% selectivity for the liquid C1 oxygenated products. This enhanced performance is attributed to the combination of one-dimensional structure and the synergistic effect from the suitable portion of Au on Pd sites, which regulates bond strength between adsorbed radicals (•OH, •OOH, •CH 3 ) and PdAu atoms, confirmed by the density function theory calculations.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Qi Si Chen,Peng Lei Cui,Jun Yang,Dong Chen,Hui Liu,Huiyan Feng,Panagiotis Tsiakaras,Pei Kang Shen
Electrochemical carbon dioxide reduction reaction (CO 2 RR) is regarded as an effective strategy to store abundant renewable energy and build a carbon neutral society. Gold (Au) and silver (Ag)-based catalysts for the effective electrochemical transformation of CO 2 to CO emerge as promising candidates. Heterogeneous nanocomposites composed of noble metals and semiconductors exhibit great potential for electrocatalytic CO 2 reduction through the electronic coupling effect at coherent interfaces. Herein, we successfully synthesize heterogeneous Ag 2 S-Au composite nanoparticles (NPs) as effective catalysts for CO production through CO 2 RR. At −0.8 V vs RHE, the heterogeneous Ag 2 S-Au nanocatalysts display a considerable CO Faradaic efficiency of 94.5%, and an appreciable CO partial current density of 9.17 mA cm −2 . Moreover, they exhibit good stability for 30 h without obvious decrease. On the basis of density functional theory (DFT) calculations, it can be made clear that the heterogeneous Ag 2 S-Au interface is energetically more beneficial to the generation of COOH* intermediate for CO 2 RR. This study provides a new application for noble metal–semiconductor nanocomposites.
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