ORCID Profile
0000-0001-6691-3986
Current Organisation
Donghua University
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Publisher: Wiley
Date: 22-07-2014
Abstract: Recent advances in direct-use plasmonic-metal nanoparticles (NPs) as photocatalysts to drive organic synthesis reactions under visible-light irradiation have attracted great interest. Plasmonic-metal NPs are characterized by their strong interaction with visible light through excitation of the localized surface plasmon resonance (LSPR). Herein, we review recent developments in direct photocatalysis using plasmonic-metal NPs and their applications. We focus on the role played by the LSPR of the metal NPs in catalyzing organic transformations and, more broadly, the role that light irradiation plays in catalyzing the reactions. Through this, the reaction mechanisms that these light-excited energetic electrons promote will be highlighted. This review will be of particular interest to researchers who are designing and fabricating new plasmonic-metal NP photocatalysts by identifying important reaction mechanisms that occur through light irradiation.
Publisher: American Chemical Society (ACS)
Date: 08-04-2013
DOI: 10.1021/JA400527A
Abstract: The intrinsic catalytic activity of palladium (Pd) is significantly enhanced in gold (Au)-Pd alloy nanoparticles (NPs) under visible light irradiation at ambient temperatures. The alloy NPs strongly absorb light and efficiently enhance the conversion of several reactions, including Suzuki-Miyaura cross coupling, oxidative addition of benzylamine, selective oxidation of aromatic alcohols to corresponding aldehydes and ketones, and phenol oxidation. The Au/Pd molar ratio of the alloy NPs has an important impact on performance of the catalysts since it determines both the electronic heterogeneity and the distribution of Pd sites at the NP surface, with these two factors playing key roles in the catalytic activity. Irradiating with light produces an even more profound enhancement in the catalytic performance of the NPs. For ex le, the best conversion rate achieved thermally at 30 °C for Suzuki-Miyaura cross coupling was 37% at a Au/Pd ratio of 1:1.86, while under light illumination the yield increased to 96% under the same conditions. The catalytic activity of the alloy NPs depends on the intensity and wavelength of incident light. Light absorption due to the Localized Surface Plasmon Resonance of gold nanocrystals plays an important role in enhancing catalyst performance. We believe that the conduction electrons of the NPs gain the light absorbed energy producing energetic electrons at the surface Pd sites, which enhances the sites' intrinsic catalytic ability. These findings provide useful guidelines for designing efficient catalysts composed of alloys of a plasmonic metal and a catalytically active transition metal for various organic syntheses driven by sunlight.
Publisher: American Chemical Society (ACS)
Date: 19-10-2023
Publisher: Wiley
Date: 2023
Abstract: Oxygen reduction reaction (ORR) and sulfur reduction reaction (SRR) play key roles in advanced batteries. However, they both suffer from sluggish reaction kinetics. Here, an interesting nitrogen doped porous carbon material that can simultaneously activate oxygen and sulfur is reported. The carbon precursor is a nitrogen containing covalent organic framework (COF), constituting periodically stacked 2D sheets. The COF structure is well preserved upon pyrolysis, resulting in the formation of edge‐rich porous carbon with structure resembling stacked holey graphene. The nitrogen containing groups in the COF are decomposed into graphitic and pyridinic nitrogen during pyrolysis. These edge sites and uniform nitrogen doping endow the carbon product with high intrinsic catalytic activities toward ORR and SRR. The COF derived carbon delivers outstanding performances when assembling as cathodes in the Li‐S and Li‐O 2 batteries. Simultaneous activation of oxygen and sulfur also enables a new battery chemistry. A proof‐of‐concept Li‐S/O 2 hybrid battery is assembled, delivering a large specific capacity of 2,013 mAh g −1 . This study may inspire novel battery designs based on oxygen and sulfur chemistry.
Publisher: Wiley
Date: 20-08-2015
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D2QI02487J
Abstract: We report an ultrathin defect-rich nickel–cobalt oxide nanosheet array, which can actively and stably catalyze oxygen evolution and reduction reactions.
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C7DT00418D
Abstract: Silver and palladium alloy nanoparticle catalysts for reductive coupling of nitrobenzene through light irradiation.
Publisher: Elsevier BV
Date: 10-2014
Publisher: American Chemical Society (ACS)
Date: 20-02-2023
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D2SE01783K
Abstract: A heterojunction CdS/TiO 2 nanofiber monolithic photocatalyst sheet was developed via facile in situ hydrothermal growth on Ti foil. The photocatalyst sheet can greatly enhance photocatalytic H 2 production.
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1TA08770C
Abstract: The hydrogen evolution activity of Ga-doped La 5 Ti 2 Cu 0.9 Ag 0.1 O 7 S 5 (Ga-LTCA) was boosted by loading a Rh cocatalyst having uniform dispersion and intimate contact.
Publisher: Elsevier BV
Date: 07-2017
Publisher: Royal Society of Chemistry (RSC)
Date: 2016
DOI: 10.1039/C5GC01726B
Abstract: The photocatalytic reduction of nitroaromatics on Ag–Cu alloy NPs can maintain the selectivity to azoxy compounds, whereas Ag NPs mainly obtain azo compounds.
Publisher: American Chemical Society (ACS)
Date: 22-08-2021
Publisher: American Chemical Society (ACS)
Date: 17-06-2016
Abstract: Hydrotalcite (HT)-based materials are usually applied to capture anionic pollutants in aqueous solutions. Generally considered anion exchangers, their ability to capture radioactive cations is rarely exploited. In the present work, we explored the ability of pristine and calcined HT getters to effectively capture radioactive cations (Sr(2+) and Ba(2+)) which can be securely stabilized at the getter surface. It is found that calcined HT outperforms its pristine counterpart in cation removal ability. Meanwhile, a novel anion removal mechanism targeting radioactive I(-) is demonstrated. This approach involves HT surface modification with silver species, namely, Ag2CO3 nanoparticles, which can attach firmly on HT surface by forming coherent interface. This HT-based anion getter can be further used to capture I(-) in aqueous solution. The observed I(-) uptake mechanism is distinctly different from the widely reported ion exchange mechanism of HT and much more efficient. As a result of the high local concentrations of precipitants on the getters, radioactive ions in water can be readily immobilized onto the getter surface by forming precipitates. The secured ionic pollutants can be subsequently removed from water by filtration or sedimentation for safe disposal. Overall, these stable, inexpensive getters are the materials of choice for removal of trace ionic pollutants from bulk radioactive liquids, especially during episodic environmental crisis.
Publisher: Elsevier BV
Date: 07-2012
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1TA01162F
Abstract: A well-dispersed Pt cocatalyst obtained using Na as a promoter provides enhanced photocatalytic hydrogen evolution over BaTaO 2 N under visible light.
Publisher: Elsevier BV
Date: 05-2021
Publisher: Georg Thieme Verlag KG
Date: 17-05-2016
Publisher: Wiley
Date: 02-2015
Publisher: Elsevier BV
Date: 2011
Publisher: Elsevier BV
Date: 07-2021
Publisher: Elsevier BV
Date: 07-2010
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C7CY02291C
Abstract: Selective hydrogenation of various chemical bonds, such as CC, CC, CO, NO, and CN, is efficiently driven by visible light over a supported gold nanoparticle (AuNP) photocatalyst under mild reaction conditions.
Publisher: Wiley
Date: 07-02-2014
Abstract: Supported nanoparticles (NPs) of nonplasmonic transition metals (Pd, Pt, Rh, and Ir) are widely used as thermally activated catalysts for the synthesis of important organic compounds, but little is known about their photocatalytic capabilities. We discovered that irradiation with light can significantly enhance the intrinsic catalytic performance of these metal NPs at ambient temperatures for several types of reactions. These metal NPs strongly absorb the light mainly through interband electronic transitions. The excited electrons interact with the reactant molecules on the particles to accelerate these reactions. The rate of the catalyzed reaction depends on the concentration and energy of the excited electrons, which can be increased by increasing the light intensity or by reducing the irradiation wavelength. The metal NPs can also effectively couple thermal and light energy sources to more efficiently drive chemical transformations.
Publisher: Royal Society of Chemistry (RSC)
Date: 2016
DOI: 10.1039/C6CC05186C
Abstract: Non-plasmonic Pd NPs and Pt NPs exhibit superior visible light photocatalytic activity and distinctly different product selectivity in the oxidation of aliphatic alcohols.
Publisher: American Chemical Society (ACS)
Date: 17-08-2022
DOI: 10.1021/ACS.INORGCHEM.2C02359
Abstract: A two-dimensional (2D) Janus film with self-assembled gold nanoparticles (AuNPs) is a class of fascinating materials that may offer unprecedented opportunities to realize erse applications due to their two distinct faces with anisotropic properties. In this work, we report a novel, straightforward strategy for the preparation of a bilayer coordination nanosheet (CONASH)/AuNP Janus film, where the CONASH features infinite trinuclear gold(I) pyrazolate cyclic complexes with electron-accepting viologen as bridges. The bilayer film has visible light absorption and redox properties and showcased promising photocatalytic H
Publisher: Elsevier BV
Date: 11-2016
Publisher: Elsevier BV
Date: 2012
Publisher: American Chemical Society (ACS)
Date: 23-05-2017
DOI: 10.1021/ACS.JPCLETT.7B00941
Abstract: By investigating the action spectra (the relationship between the irradiation wavelength and apparent quantum efficiency of reactions under constant irradiance) of a number of reactions catalyzed by nanoparticles including plasmonic metals, nonplasmonic metals, and their alloys at near-ambient temperatures, we found that a photon energy threshold exists in each photocatalytic reaction only photons with sufficient energy (e.g., higher than the energy level of the lowest unoccupied molecular orbitals) can initiate the reactions. This energy alignment (and the photon energy threshold) is determined by various factors, including the wavelength and intensity of irradiation, molecule structure, reaction temperature, and so forth. Hence, distinct action spectra were observed in the same type of reaction catalyzed by the same catalyst due to a different substituent group, a slightly changed reaction temperature. These results indicate that photon-electron excitations, instead of the photothermal effect, play a dominant role in direct photocatalysis of metal nanoparticles for many reactions.
Publisher: American Chemical Society (ACS)
Date: 30-01-2015
DOI: 10.1021/JA511619C
Abstract: Selective oxidation of aliphatic alcohols under mild and base-free conditions is a challenging process for organic synthesis. Herein, we report a one-pot process for the direct oxidative esterification of aliphatic alcohols that is significantly enhanced by visible-light irradiation at ambient temperatures. The new methodology uses heterogenerous photocatalysts of gold-palladium alloy nanoparticles on a phosphate-modified hydrotalcite support and molecular oxygen as a benign oxidant. The alloy photocatalysts can absorb incident light, and the light-excited metal electrons on the surface of metal nanoparticles can activate the adsorbed reactant molecules. Tuning the light intensity and wavelength of the irradiation can remarkably change the reaction activity. Shorter wavelength light (<550 nm) drives the reaction more efficiently than light of longer wavelength (e.g., 620 nm), especially at low temperatures. The phosphate-exchanged hydrotalcite support provides sufficient basicity (and buffer) for the catalytic reactions thus, the addition of base is not required. The photocatalysts are efficient and readily recyclable. The findings reveal the first ex le of using "green" oxidants and light energy to drive direct oxidative esterification of aliphatic alcohols under base-free, mild conditions.
Publisher: Elsevier BV
Date: 2012
Publisher: Springer Science and Business Media LLC
Date: 2021
Publisher: American Chemical Society (ACS)
Date: 22-01-2019
Publisher: American Chemical Society (ACS)
Date: 12-02-2016
Publisher: Elsevier BV
Date: 09-2023
Publisher: Royal Society of Chemistry (RSC)
Date: 26-06-2014
DOI: 10.1039/C4GC00588K
Publisher: American Chemical Society (ACS)
Date: 07-2021
DOI: 10.1021/JACS.1C04861
Publisher: Elsevier BV
Date: 11-2019
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D0CY02311F
Abstract: Direct photoexcitation of metal nanoparticles (NPs) can induce selective chemical reactions that are difficult to achieve with thermal energy.
Publisher: American Chemical Society (ACS)
Date: 08-08-2014
DOI: 10.1021/JP505552V
Publisher: American Chemical Society (ACS)
Date: 30-04-2014
DOI: 10.1021/CS5000284
Publisher: American Chemical Society (ACS)
Date: 24-02-2021
Publisher: American Chemical Society (ACS)
Date: 26-09-2018
Publisher: American Chemical Society (ACS)
Date: 29-10-2020
DOI: 10.26434/CHEMRXIV.13152953.V1
Abstract: In this paper, we developed the fabrication of a plasmonic near-perfect absorber with a dense, uniform monolayer of AuPd alloyed nanoparticles as the absorbing layer. The nanoparticles were prepared by dewetting thin films ( nm) of each metal on a dielectric surface and extensive characterization confirmed the lack of other bimetallic phases. Plasmonic near-perfect absorbers containing an alloyed nanoparticle layer demonstrated both strong on-resonance absorption of incident light (up to 97%) and an improved photocatalytic response, compared to either monometallic derivative, for the photoelectrochemical reduction of water.
No related grants have been discovered for Qi Xiao.