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CHEMICAL PHYSICS LETTERS · 2015 · IF 1.897

Selective plasmon driven surface catalysis in metal triangular nanoplate-molecule-film sandwich structure

Yanna Yang,Shuxia Wang,Zhen Zhang,Yingzhou Huang,Guo Chen,Hua Wei,Weijia Wen

Combined with surface enhanced Raman scattering (SERS) and finite difference time-domain (FDTD) method, the plasmon-driven surface catalytic (PDSC) reaction of p , p ′-dimercaptoazobenzene (DMAB) produced from 4-nitrobenzenethiol (4NBT) or P-aminothiophenol (PATP) in Au triangular nanoplate-molecule-film sandwich structure is investigated. The disparity of SERS spectra at different positions on Au triangular nanoplate indicates that the surface catalysis is selective performed at some particular regions, which change along with the polarization direction of the incident laser. Furthermore, this selective surface catalysis phenomenon has also been confirmed by the simulated electric field distribution using FDTD method. Our results enlarge the metal nanostructure of PDSC reactions and provide a useful help to study the SERS and surface catalysis.

CAS / MDL: 1193-02-8 1849-36-1
研究领域: 材料科学 · 光学 · 催化化学
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Water Cycle · 2022 · IF 0

A bifunctional nanocrystal surface: Integration of slow release of copper cations and providing active catalytical sites

Yue Zhang,Zheng Zhou,Haixiang Han,Chunhua Xu

Nanoparticles represent an interesting platform that demonstrates properties absent from bulk materials. Although the employment of nanoparticles for environmental remediation has attracted tremendous attentions in both scientific research and industrial applications, there is still a huge gap between the clear mechanism understandings and their deliverable activities due to the complex reaction kinetics. Herein, we report the synthesis of high-quality, monodispersed Cu 7 S 4 nanoparticles as a model nano system to investigate the degradation mechanism of organic pollutants. The morphology, chemical composition and atomic structure of the as-prepared Cu 7 S 4 have been characterized by Transmission Electron Microscope (TEM), X-ray photoelectron spectroscopy (XPS), X-ray powder diffractometer (XRPD) and Fourier transform infrared spectra (FT-IR). In addition, it is revealed that the Cu 7 S 4 particles can effectively degrade organic pollutants, like Orange I and Orange II through a slow and controllable release of Cu cations process coupled with surface catalysis. The detailed study shows that the small amounts of released Cu cations from Cu 7 S 4 nanoparticles are first coordinated with the organic pollutants and the resultant complexes are then degraded on the surface of nanoparticles in the presence of H 2 O 2 .

研究领域: 环境科学 · 材料科学 · 化学
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS · 2022 ·Vol. 24 ·期 45 ·27900-27907 · IF 3.945

Probing catalytic reduction on the surface of Au nanoparticles by second-harmonic generation and two-photon luminescence

Shan Xue,Shun-Li Chen,Qunhui Yuan,Wei Gan

The catalytic reduction of aromatic nitro compounds by metallic nanoparticles in the presence of sodium borohydride (NaBH4) has been widely studied as model reactions. However, the reaction mechanisms still need further investigations. For example, the origin of the induction time that has often been observed is still controversial. Here, we demonstrated that such catalytic reduction reactions on the surface of colloidal gold nanoparticles (AuNPs) may be inspected by the second-harmonic generation (SHG) and two-photon luminescence (TPL) emission from AuNPs. It was revealed that the SHG and TPL signals from AuNPs were sensitive to the substitution of citrate by active hydride species derived from the hydrolysis of NaBH4. Based on the UV-vis spectroscopy analyses and monitoring the SHG/TPL signals, the induction time in the catalytic reaction of 4-nitrothiophenol was revealed to originate from the hindered adsorption of hydride on the gold surface. This work demonstrated that SHG and TPL can provide a new approach for detecting active hydrides on the surface of metallic nanoparticles in colloids.

研究领域: 化学 · 纳米科技 · 光学
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ADVANCED MATERIALS · 2025 · IF 26.8

Pressure-Assisted Ni 3d–S 3p Hybridization within Targeted In–S Layer for Enhanced Photocatalytic Hydrogen Production

Bo Shao,Tianyun Liu,Deng-Bing Li,Linxing Meng,Jianyuan Wang,Wei Zhai,Liang Li

Solar-driven hydrogen production is significant for achieving carbon neutrality but is limited by unsatisfactory surface catalytic reaction kinetics. Layer regulation can impact carrier transmission or catalytic behavior, but the specific effects on the oxygen or hydrogen evolution reaction (OER or HER) remain unclear, and atomic layer level modulation for maxing HER is challenging. Here the distinct roles of modulated Zn–S or In–S surface layers in ZnIn 2 S 4 (ZIS) for the OER and HER, respectively, are disentangled. Moreover, the extensive characterizations and computational results demonstrate that stressful environments enable individual modulation and introduce Ni into the surface In–S layer rather than the easily alterable Zn–S layer, creating deeper hybridized electronic states of Ni 3 d –S 3 p , optimizing H * adsorption/desorption, and maximizing surface catalytic benefits for the HER. Consequently, the optimized ZIS exhibited a photocatalytic hydrogen production rate of up to 18.19 mmol g −1 h −1 , ≈32 times higher than pristine ZIS. This investigation expands the application scenarios of ultrasonic technology and inspires other precise control types, such as defects and crystal plane engineering, etc.

研究领域: 材料科学 · 能源化学 · 催化反应工程
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JOURNAL OF HAZARDOUS MATERIALS · 2019 · IF 7.65

The duet of surface and radical-based carbocatalysis for oxidative destructions of aqueous contaminants over built-in nanotubes of graphite

Yuxian Wang,Jiaxin Xi,Xiaoguang Duan,Weiguang Lv,Hongbin Cao,Chunmao Chen,Zhuang Guo,Yongbing Xie,Shaobin Wang

Metal-free mesoporous graphitic frameworks with built-in nanotubes (CPGs) were synthesized via facile co-pyrolysis of cyclodextrin and a cobalt salt with subsequent acid pickling to remove the embedded metal species. Due to the high graphitic degree and built-in few-layer nanotubes, the as-synthesized carbonaceous materials possess a higher catalytic ozonation activity than that of the state-of-the-art carbon nanotubes (CNTs) and LaMnO 3 perovskite catalysts for the destruction of different aqueous contaminants. For recalcitrant oxalic acid removal, 50 mg L −1 oxalic acid was completely degraded in 20 min. Compared with other nanocarbons, the as-synthesized materials also demonstrated robust structural stability and reusability. The electron paramagnetic resonance (EPR) and selective radical quenching tests revealed that the destruction of the aqueous organics predominantly relied on surface-adsorbed complexes (O* ad and O 2 *) from activated ozone molecules. Owing to the occurrence of this surface oxidation pathway, the compatibility of the CPGs/O 3 system was significantly enhanced for treatment of real wastewater, where the inorganic anions and organic natural organic matter would inhibit radical oxidation as radical scavengers. Furthermore, by employing organics with different ionization potentials (IPs) as the target pollutants, the CPGs/O 3 system was discovered to obtain a high oxidation potential.

研究领域: 环境科学 · 材料科学
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JOURNAL OF HAZARDOUS MATERIALS · 2022 · IF 14.224

Surface-catalyzed electro-Fenton with flexible nanocatalyst for removal of plasticizers from secondary wastewater effluent

Weilu Yang,Mingshan Zhu,Wanbin Li,Guoqiang Liu,Eddy Y. Zeng

Activation of H 2 O 2 with metal-free catalysts is an efficient and environmentally benign alternative to electron-Fenton (EF) for organics degradation . In the present study, flexible nanocatalysts were synthesized with self-regulated metal oxide nanoparticles (FeOx NPs) for efficient removal of plasticizers from secondary wastewater effluent (SWE). Compared with NGr/EF and FeOx@Gr/EF systems, FeOx@NGr/EF could enhance the decay kinetics of plasticizers by 3.9–4.4 times and reduce 48–59% of the disposal cost. Reactive oxygen species tests and trapping experiments proved that the surface-catalyzed EF effectively broadened the range of solution pH. Density functional theory calculations coupled with electrochemical measurements indicated that the electron transfer rates between Fe-O-C atoms were enhanced with N-doping due to strong interactions between N-Fe bond. The synergistic effects of FeOx and N could improve the oxygen reduction activity for H 2 O 2 generation, and accelerate electron transfer between FeOx/NGr and H 2 O 2 for • OH generation, offering an alternative for wastewater treatment .

研究领域: 环境科学 · 化学工程 · 材料科学
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Catalysis Science & Technology · 2015 ·Vol. 6 ·期 9 ·2918-2929 · IF 5.426

Hierarchical shape-controlled mixed-valence calcium manganites for catalytic ozonation of aqueous phenolic compounds

Yuxian Wang,Yongbing Xie,Hongqi Sun,Jiadong Xiao,Hongbin Cao,Shaobin Wang

Catalytic ozonation has attracted intensive attention due to its efficient degradation of various organic pollutants in water. The key to a practical application is the discovery of highly effective catalysts. This study, for the first time, reports excellent performances of porous mixed-valence calcium manganite (CaMn3O6 and CaMn4O8) microspheres made of 1D nanorods in the catalytic ozonation of 4-nitrophenol. The CaMn3O6 and CaMn4O8 showed much higher activities and stabilities than manganese oxides. From a variety of advanced characterizations, the mechanism of surface catalysis was discussed in detail. Quenching reagents and electron paramagnetic resonance (EPR) spectroscopy were applied to probe the dominant reactive species in the catalytic ozonation over the calcium manganites. It was found that superoxide radicals and singlet oxygen rather than hydroxyl radicals contributed to the degradation and mineralization of 4-nitrophenol. Moreover, the effects of electron-withdrawing groups (EWG) and electron-donating groups (EDG) in the phenolic compounds on the ozonation/catalytic ozonation over the calcium manganites were investigated using phenol, p-cresol and p-chlorophenol as target pollutants.

CAS / MDL: 100-02-7
研究领域: 环境科学 · 催化化学
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SYNTHETIC METALS · 2020 · IF 3.286

Selective homocysteine detection of nitrogen-doped graphene quantum dots: Synergistic effect of surface catalysis and photoluminescence sensing

Yajie Zou,Xiaoqiang Feng,Yun Zhao,Zhiheng Wei,Wei Zhu,Menghan Zhao,Ting Wang,Zhiduo Liu,Shiwei Tang,Gang Wang,Qinglei Guo,Da Chen

As a new photoluminescence functional material, graphene quantum dots have aroused widely entertaining. However, the complicated surficial chemistry micro-circumstance of graphene quantum dots hinders the further study of graphene quantum dots. In this paper, we demonstrate that the selectivity and sensitivity photoluminescence (PL) detection of homocysteine based on the synergistic effect of surface catalysis and photoluminescence sensing for nitrogen-doped graphene quantum dots (N-GQDs). Due to the localized superacid microenvironment of N-GQDs, the homocysteine cyclized into homocysteine thiolactone efficiently and selectively. Meanwhile, the aromatic N in N-GQDs adsorbs homocysteine thiolactone selectively. The following static quenching results in the outstanding selectivity and sensitivity PL quenching of N-GQDs with the presence of homocysteine. The detection limit is 5 × 10 −11 M, which is much lower than most reported detection methods. We also demonstrate that N-GQDs are able to display a PL response to homocysteine in the living cells.

研究领域: 生物化学 · 纳米医学 · 分析化学
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Journal of Energy Chemistry · 2025 · IF 14.9

Substituent engineering of edge-modified cobalt polyphthalocyanine for optimizing near-infrared photocatalytic imines synthesis: dual regulation of surface catalytic reactions

Hao Chen,Hao Jiang,Mei Yan,Chongshen Guo

The photocatalytic oxidative coupling of amines has emerged as a promising alternative for imine production. Nevertheless, enhancing the photocatalytic activity of conjugated organic polymers (COP) still faces significant challenges, particularly in near-infrared (NIR) driven photocatalytic activity, charge separation efficiency, adsorption, and activation of amine molecules. Here, we tackled these challenges by modulating the internal electronic states of cobalt phthalocyanine polymers (C-CoPPc- x ) through edge-substituted modification with various electron-donating or electron-withdrawing groups. The built-in electric field (B-IEF) and Lewis acidity of metal sites are significantly influenced by such an edge-substituted modification, which further results in an adjustable separation efficiency of photogenerated charges and the adsorption/activation behavior of benzylamine. By optimizing the surface catalytic reactions of COP, the methoxy-edge-modified polymer demonstrated a superior performance with an amine yield of 4.32 mmol g −1 under NIR irradiation, surpassing the performance of many reported photocatalysts even under ultraviolet (UV) or visible light. This work underscores the substantial impact of minor substituent modifications on both the separation of photogenerated charge carriers and the adsorption/activation of amine molecules in the photocatalytic process, and provides valuable insights for enhancing the photocatalytic performance of COP in diverse applications.

研究领域: 光催化 · 高分子化学 · 有机合成 · 材料科学 · 表面工程
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Scientific Reports · 2015 ·Vol. 5 ·期 1 ·1-8 · IF 5.578

Electromagnetic field redistribution induced selective plasmon driven surface catalysis in metal nanowire-film systems

Pan Liang,Huang Yingzhou,Yang Yanna,Xiong Wen,Chen Guo,Su Xun,Wei Hua,Wang Shuxia,Wen Weijia

For the novel interpretation of Raman spectrum from molecule at metal surface, the plasmon driven surface catalysis (PDSC) reactions have become an interesting topic in the research field of surface enhanced Raman scattering (SERS). In this work, the selective PDSC reactions of p,p’-dimercaptoazobenzene (DMAB) produced from para-aminothiophenol (PATP) or 4-nitrobenzenethiol (4NBT) were demonstrated in the Ag nanowires dimer-Au film systems. The different SERS spectra collected at individual part and adjacent part of the same nanowire-film system pointed out the importance of the electromagnetic field redistribution induced by image charge on film in this selective surface catalysis, which was confirmed by the simulated electromagnetic simulated electro- magnetic field distributions. Our result indicated this electromagnetic field redistribution induced selective surface catalysis was largely affected by the polarization and wavelength of incident light but slightly by the difference in diameters between two nanowires. Our work provides a further understanding of PDSC reaction in metal nanostructure and could be a deep support for the researches on surface catalysis and surface analysis.

CAS / MDL: 104-96-1
研究领域: 材料科学 · 物理化学 · 光谱学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Simultaneous enhancement of charge transfer and surface catalysis through a polymetallic oxide cocatalyst on BiVO4 photoanodes for highly efficient and stable water oxidation

Yuchen Zhou,Hongxing Li,Peng Guo,Yu Zhang,Peng Zhou

The rate-determining oxygen evolution reaction (OER) always limits the high-efficient conversion of solar energy to green hydrogen fuels through photoelectrocatalytic or photocatalytic water splitting. The high catalytic overpotential and the instability of catalytic center are commonly regarded as the primary factors contributing to the low rate of OER, remaining to be a challenge in the field of water splitting. Herein, a polymetallic oxide cocatalyst (Mo-MnO y /FeCoNiO x ) with well-defined electronic and catalytic properties is designed on BiVO 4 photoelectrode for highly efficient and stable photoelectrocatalytic water oxidation. The experimental characterization demonstrates that the dual-layer design of Mo-MnO y /FeCoNiO x can significantly optimizes the electronic property of MnO y and FeCoNiO x components, boosting the photogenerated charge transfer between Mo-MnO y /FeCoNiO x cocatalyst and BiVO 4 photoelectrode. The density functional theory (DFT) simulation reveals that the Mo sites in Mo-MnO y layer can activate the neighboring surface Mn sites instead of directly serving as the catalytic center, thereby establishing these Mn sites as primary active centers for achieving stable OER. The developed Mo-MnO y /FeCoNiO x /BiVO 4 photoelectrode exhibits a current density of 6.18 mA cm −2 with an excellent stability for 30 h at 1.23 V RHE under 1 sun irradiation, exhibiting the excellent activity and durability. This work sheds light on design of high-performance multiple-component water-oxidation cocatalyst on photoanode.

研究领域: 光电化学 · 催化 · 材料科学 · 能源转换
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Plasmonics · 2015 ·Vol. 11 ·期 3 ·909-915 · IF 2.238

Ascertaining Plasmonic Hot Electrons Generation from Plasmon Decay in Hybrid Plasmonic Modes

Wang Shuxia,Wang Hui,Liu Ting,Huang Yingzhou,Chen Guo,Wei Hua,Su Xun,Zeng Xiping,Xia Zengzilu,Wen Weijia,Sun Mengtao

In the propagating process along metal surface, surface plasmon polaritons (SPPs) mainly decay into thermal loss or release into photons, while a part of them were converted into electrons with high energy termed as hot electrons, which have great significance in photonics and electronics. In this work, the generation of plasmonic hot electrons was ascertained in the nanoparticle-film system through plasmon-driven surface catalysis (PDSC) reactions. The surface-enhanced Raman scattering (SERS) spectra of p,p'-dimercaptoazobenzene (DMAB) catalyzed by 4-nitrobenzenethiol (4NBT) experimentally demonstrated the essential catalysis electrons were generated in this hybrid plasmon mode. The results pointed out the priority of plasmonic hot electron generation in the dimer-film gap compared to the monomer-film gap which was analyzed by the surface electric and charge distribution. Furthermore, the SERS spectra of 4NBT in the metal nanoparticle-dielectric film system confirmed the necessity of hybrid plasmon mode in the generation of plasmonic hot electrons in the nanoparticle-film system. Because of the simple configuration and convenient fabrication of nanoparticle-film system, the work on this hybrid plasmon mode has a significant role in promoting the application of plasmonic hot electrons.

研究领域: 纳米光子学 · 等离激元学 · 表面科学 · 催化化学 · 分子光学 · 材料物理 · 半导体器件
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