Photogenerated carrier behavior at a gas-solid interface for CO2 adsorption on Cs2AgBiBr6 nanocrystals.

Photogenerated carrier behavior at a CO2/Cs2AgBiBr6 quantum dot (QD) interface is investigated. In situ photovoltage spectra reveal electron transfer from the Cs2AgBiBr6 QDs to CO2. Moreover, this carrier transfer prefers Bi3+ sites (over Ca+ and Ag+ sites) due to them exhibiting the lowest adsorption energy (Eads = -0.125 eV) and CO2-Bi3+ interactions being more stable.

SERS monitoring of photoinduced-enhanced oxidative stress amplifier on Au@carbon dots for tumor catalytic therapy.

Currently, artificial enzymes-based photodynamic therapy (PDT) is attractive due to its efficient capacity to change the immunosuppressive tumor microenvironment (TME). It is of great significance to study the therapeutic mechanism of novel artificial enzymes in TME through a monitoring strategy and improve the therapeutic effect. In this study, Au@carbon dots (Au@CDs) nanohybrids with a core-shell structure are synthesized, which not only exhibit tunable enzyme-mimicking activity under near-infrared (NIR) light, but also excellent surface-enhanced Raman scattering (SERS) properties. Therefore, Au@CDs show a good capability for monitoring NIR-photoinduced peroxidase-like catalytic processes via a SERS strategy in tumor. Moreover, the Au@CDs deplete glutathione with the cascade catalyzed reactions, thus elevating intratumor oxidative stress amplifying the reactive oxygen species damage based on the NIR-photoinduced enhanced peroxidase and glutathione oxidase-like activities, showing excellent and fast PDT therapeutic effect promoted by photothermal property in 3 min, finally leading to apoptosis in cancer cells. Through SERS monitoring, it is further found that after removing the NIR light source for 33 min, the reactive oxygen species (ROS) activity of the TME is counteracted and eliminated due to the presence of glutathione. This work presents a guidance to rationally design of artificial enzyme for ROS-involved therapeutic strategies and a new spectroscopic tool to evaluate the tumor catalytic therapy.

Photon-recycling effect in perovskites for photovoltaic applications: a Monte Carlo study.

Photon recycling has been shown to play an important role in the optoelectronic properties and device performance of perovskite solar cells recently. However, there lacks an analytical method to accurately predict the dynamics of charge carriers and photons and the device performance with photon recycling due to the complexity of multiple electron-photon conversion processes involved in photon recycling. We propose a model based on the Monte Carlo simulation method that combines charge carrier diffusion and photon radiation transport to analyze the effects of photon recycling on electron-photon dynamics and device performance of perovskite solar cells. We show that the carrier lifetime can be significantly boosted by photon recycling in the radiative limit, which yields a 37 meV increase in the open-circuit voltage for a 500 nm thick perovskite solar cell. Our results provide insights for the working mechanisms of perovskite solar cells, and the new model can be further applied to other types of solar cells with photon recycling.

Accurate SERS monitoring of the plasmon mediated UV/visible/NIR photocatalytic and photothermal catalytic process involving Ag@carbon dots.

The excited carriers (electrons and holes) and heat energy that originate from plasmonic metal nanomaterials are crucial to the enhancement of the photocatalytic performance. In this study, an Ag@carbon dots (Ag@CDs) hybrid has been prepared with excellent Fenton-like photocatalytic and photothermal conversion properties for catalyzing H2O2 to generate hydroxyl radicals (˙OH) for the degradation of crystal violet (CV) dye under full solar spectrum irradiation based on a unique plasmon effect. We have obtained some intrinsic kinetics information, including the reaction rate and apparent activation energy on the surface of the Ag@CDs, through a surface-enhanced Raman scattering strategy to investigate the contributions made by photocatalytic and photothermal effects in the plasmon mediated reaction under irradiation from ultraviolet (UV)/visible/near-infrared (NIR) light. In the visible light region, the Ag@CDs + H2O2 system exhibits the fastest apparent reaction rate owing to the involvement of a large number of hot carriers, which are generated by the strongest plasmon effect, and the presence of the photothermal effect mediated by the plasmonic effect. As the wavelength of the illumination blue-shifts to the UV region, the plasmon effect is weakened, resulting in a decrease in the number of hot carriers. Furthermore, the hot carriers will not be further thermalized because of interband transitions. In addition, the catalytic performance of Ag@CDs in the NIR region is almost dominated by the photothermal effect. This work provides deep insights into understanding the plasmon-mediated photocatalytic mechanism of the Ag@CDs hybrid.

Ultra-sensitive SERS detection, rapid selective adsorption and degradation of cationic dyes on multifunctional magnetic metal-organic framework-based composite.

In-situ and real-time ultra-sensitive monitoring for the degradation process of environmental pollutants is always an important issue of concern to many people. Herein, a multifunctional magnetic metal-organic framework (MOF)-based composite has been successfully constructed and applied in monitoring the disposal of cationic dyes. Owing to its particular MOFs shell and internal gold particles, the composite can be used as an efficient SERS substrate to ultra-sensitively detect the cationic dyes. Furthermore, the prepared MOF-based composite is also a peroxidase-like nanozyme, which can catalytically degrade the adsorbed cationic dyes. Additionally, the magnetic core in the MOF-based composite offers a good magnetic separation capacity, which makes a facile and rapid separation of the catalyst from the reacted solution for recyclability. This work has provided a new way to monitor the catalytic degradation process by SERS technique in the co-existence of catalyst and dye molecules in the reaction system, which can effectively eliminate the absorption of the catalyst compared with the UV-vis technique, showing promising applications in in-situ and real-time pollution disposal monitoring.

Highly efficient core-shell Ag@carbon dot modified TiO2 nanofibers for photocatalytic degradation of organic pollutants and their SERS monitoring.

In the present study, a novel hybrid nanomaterial composed of core-shell structured Ag@carbon dot (CD) modified TiO2 nanofibers (NFs) was successfully fabricated via a simple two-step strategy for the first time. Herein, the Ag@CDs-TiO2 NFs are demonstrated to be an efficient SERS substrate. The strong LSPR-induced electromagnetic enhancement (EM) by Ag@CDs NPs and efficient charge transfer (CT) effect between Ag@CDs and TiO2 NFs synergistically contribute to the excellent SERS enhancement. In addition, the Ag@CDs-TiO2 NFs exhibit enhanced photocatalytic activity regarding the organic pollutant degradation under visible light irradiation because of the enhanced light absorption and improved separation of photo-generated electron-hole pairs. Thus, this new nanocomposite can be used as a sensitive SERS substrate for determining the catalytic activity and reaction kinetics during the photodegradation of methylene blue (MB). Compared with UV-vis spectroscopy, the SERS technique enables more accurate monitoring of the changes of adsorption molecules and actual catalytic process on the surface of the catalyst. These results are significant for the development of metal or semiconductor-based catalysts for ensuring optoelectronic, energy and environmental applications.