Journal of Materials Chemistry B
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2022
·Vol. 10
·期 23
·4501-4508
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IF 7.571
Xi Xiao,Bingzhu Zheng,Qiang Zheng,Zijie Lu,Dong Cen,Xiujun Cai,Xiang Li,Renren Deng
Peroxynitrite anion (ONOO−), a product derived from reaction between reactive oxygen species (ROS) and nitric oxide (NO), is considered to be a more toxic reactive species than most ROS for cancer photodynamic therapy (PDT). To promote the PDT effect, a viable method is to develop rational strategies for efficient ONOO− generation at targeted tumor sites. Herein, a heterostructure nanocomposite containing ZnO-coated lanthanide nanoparticles (LnNPs) is reported for ONOO−-based PDT. In this nanocomposite, Nd3+-doped LnNPs are employed to realize efficient NIR-light-triggered ROS generation by activating the triplet state of chlorin-e6 (Ce6) photosensitizers via a direct lanthanide-to-triplet sensitization mechanism. Meanwhile, ZnO in the composite catalyzes the decomposition of S-nitrosoglutathione (GSNO) to generate NO in the tumor microenvironment. The coupled system allows the combination of photo-induced ROS and NO to produce ONOO−, leading to drastically promoted cancer cell apoptosis and tumor growth inhibition. This study establishes a new apoptosis-inducing PDT agent, which is potentially active in drug resistant malignancies.
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ACS Sustainable Chemistry & Engineering
·
2023
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IF 8.4
Ting Zhu,Bo Wu,Jing Xie,Hongran Yang,Weibin Zhang,Yanyan Sun
Hierarchical structured p–n heterojunctions comprising cuprous oxide nanowire cores (Cu2O NW) and CoFe-layered double hydroxide (CoFe LDH) nanosheet shells on copper foam (CF) substrates were constructed by in situ wet–chemical reactions with subsequent electrodeposition. The synergistic effect of the superior light-harvesting ability of Cu2O and the built-in electric field generated by the Cu2O/CoFe LDH p–n heterojunction is verified to facilitate the efficient separation of photogenerated electrons and holes by promoting the rapid transfer of photogenerated charge carriers. Benefiting from the advantages above, the optimal CF@Cu2O NW/LDH-3 exhibits light-enhanced catalysis toward the hydrogen evolution reaction (maximum enhancement of 14.4%) and oxygen evolution reaction (maximum enhancement of 7.4%) for water splitting. Moreover, the alkaline electrolytic cell based on the optimal CF@Cu2O NW/LDH-3 requires an operating potential of only 1.62 V to drive a high current density of 100 mA cm–2 under illumination. Meanwhile, a current density retention of up to 91.62% can be reserved after a stability test for 24 h. This work provides ideas for the design of transition metal-based catalytic materials for photodriven electrochemical water splitting.
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CHEMOSPHERE
·
2023
·
IF 8.8
Beizhao Chen,Xun Liu,Bei Liu,Qi Han,Li Li,Li Wang,Yufei Shu,Linlin Zang,Wenlei Zhu,Zhongying Wang
Carbon nitride (CN) is an emerging 2D non-metal semiconductor material that could be used in photocatalysis and advanced oxidation processes (AOPs) for pollutants degradation . The radical-induced degradation by CN in photocatalysis or photo-assisted AOPs was widely reported in previous studies. Nevertheless, how the non-radical degradation by CN materials could be achieved under irradiation is neither well understood nor controlled. In this work, crystalline carbon nitride (CCN) was synthesized via a facile molten-salt method, and used to activate peroxymonosulfate (PMS) under visible light (>420 nm) to selectively and efficiently degrade tetracycline (TC). Compared to the traditional polymeric carbon nitride (PCN), CCN was found to be a superior PMS activator with the assistance of visible light, which was ascribed to the increased crystallinity of CN tri-s-triazine units and the increased number of catalytic sites, thereby optimizing the photoelectric properties. The activation performance could be further improved by copper loading, with TC degradation rate nearly six times more than that of PCN. EPR trapping and quenching tests showed that singlet oxygen ( 1 O 2 ) was the dominant reactive oxygen species in the CCN/PMS/visible light system, attributing to the increased graphitic N sites and formation of electron-deficient C in C–N bonding between neighboring tri-s-triazine units upon crystallinity elevation in CCN. In contrast to the conventional radical-based photocatalysis and AOP processes, the visible light-assisted non-radical AOP degradation was highlighted for the selectivity and the remarkable resistance to the impacts of background inorganic anions or natural organic matter (up to 10 mg/L) in the actual water matrix. This work revealed the 1 O 2 generation mechanism by CN-based materials under the joint assistance of visible light illumination and crystallinity elevation, and its excellent removal performance demonstrates the great potential of CCN-based materials in the practical wastewater treatment .
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CATALYSIS LETTERS
·
2023
·
IF 2.8
Chen Feng,Jiao Peixin,Zhao Caixian
Single-atom photocatalysts exhibit outstanding performance in energy and environmental photocatalysis, due to their exceptional capabilities in enhancing light-harvesting, charge transfer dynamics, and surface reactions. The key to preparing single-atom photocatalysts lies in developing an appropriate metal-support that can prevent aggregation or sintering during synthetic procedures. In this work, a Co(II)-urea complexe in-situ formed in melamine was employed as single-atom Co precursors to synthesize an efficient single-atom Co decorated P doped g-C 3 N 4 (Co/PCN) photocatalyst. The high-angle annular dark field transmission electron microscope (HAADF-TEM) results indicated abundant Co single atoms were immobilized in the g-C 3 N 4 matrix. Under visible-light irradiation, the as-prepared photocatalysts show remarkably enhanced photocatalytic performance. Especially, loaded with 1.5 wt% single atoms Co, the optimized Co/PCN exhibits H 2 evolution of 892.5 µmol g −1 h −1 , which is 33 times higher than that of PCN, and even twice as much as that of Pt-loaded g-C 3 N 4 (Pt/PCN). The enhanced photocatalytic activity is ascribed to the synergistic effect between single-atom Co and P doping, which facilitates efficient light harvesting, charge separation, and migration. It is believed that this study paves a new avenue for developing high-efficiency single-atom photocatalysts. Graphical Abstract
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ADVANCED FUNCTIONAL MATERIALS
·
2023
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IF 19
Jinquan Liu,Liangliang Xu,Qixiao Ji,Longfei Chang,Ying Hu,Qingyu Peng,Xiaodong He
Phototropism and self-oscillation are both self-regulating intelligent movements of biological organisms. However, realizing these intelligent movements in one same artificial actuation system remains a great challenge. Here, by introducing dynamic light-mechanical interaction, a MXene-based actuator is designed and fabricated that can generate unique self-adaptive light-driven actuation from the equilibrium state of phototropic deformation to self-oscillation. The actuator can autonomously track the incident light, showing a sunflower-like phototropism. Moreover, by simply installing a load on the actuator to induce self-shadowing-enabled negative feedback loop, it can carry the load to continuously oscillate under constant light irradiation, with a frequency of 6.5 Hz, an amplitude of 2.6 mm, and a load-to-weight ratio value of 4.7. The oscillation frequency and amplitude can be further adjusted by the incident light power, actuator length, and weight of the installed load. This oscillator can serve as an intelligent light-powered motor platform. By installing diverse accessories with different functions on the oscillator, it can realize various applications, including information transmission, light-induced power generation, bionic motions, and multi-mode intelligent switches. These results provide a simple and versatile strategy for designing a self-adaptive oscillator driven by light and show the prospect of the oscillator in light-powered engines and smart machinery systems.
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Physica Status Solidi-Rapid Research Letters
·
2023
·Vol. 18
·期 2
·2300350
·
IF 2.8
Xueqing Ma,Tianrui Zhou,Yunluo Wang,Jianghua Wu,Zesheng Pan,Yuntian Fu,Jingshan Hou,Wan Jiang,Lianjun Wang,Haijie Chen
Copper halides have attracted extensive interest because of the merits of environmental friendliness, low lost, and superior optoelectronic properties. However, the stability issue heavily hinders their commercial application. Herein, the successful synthesis of copper chlorine in glass using melting-quenching method under vacuum condition is reported. By introducing CuCl into the glass matrix (CuCl@glass), the as-fabricated samples emit white or yellow light, which depends on the ratios of CuCl:glass. The maximum values of the photoluminescence quantum yield are found to be 37% and 26%, respectively. With the addition of CsCl, CsCu 2 Cl 3 , and Cs 3 Cu 2 Cl 5 phases form in the glass, leading to the phosphor-in-glass which emits green light. A maximum luminous yield of 74% is achieved. Based on the synthesized samples, light-emitting diodes are successfully prepared by the remote packaging technology, and the utilization of the as-obtained composites for anticounterfeiting application is realized. Herein, an effective approach for the preparation of lead-free halide perovskite@glass composites is provided, opening up potential commercial applications.
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Halizati Abulimiti,Reziwanguli Yantake,Aierpati Taximaimaiti,Taximaiti Yusufu,Aierken Sidike
Currently, there is a cyan gap in white light-emitting diodes (LEDs) manufactured by combining near-ultraviolet (NUV) chips with tricolour (blue/green/red) phosphors, resulting in a poor colour rendering index (Ra). Broadband blue-cyan phosphors contain blue, cyan and green luminescent components that complement the cyan gap. In this paper, feldspar-structured Ba 0.92- x Sr x Al 2 Si 2 O 8 :0.08Eu 2+ ( x = 0–0.5) phosphors were prepared by a high-temperature solid-phase method and a cation substitution strategy. A phase transition was achieved by varying the concentration of x , which resulted in the formation of two luminescent centres and a 10.33-fold enhancement of the luminescence intensity for Ba 0.92 Al 2 Si 2 O 8 :0.08Eu 2+ . The colour of the emission changed from the original green to blue-cyan, and the strongest emission peak with a half-height width of 94.5 nm was observed at a Sr 2+ concentration of 0.3 (30%) and covered the blue, cyan and green wavelength ranges (390–600 nm). The experimental value of the optical band of the substrate is 5.71 eV, and the luminous intensity of the Ba 0.62 Sr 0.3 Al 2 Si 2 O 8 :0.08Eu 2+ sample at 150 °C was 91.3% of that at room temperature. Ba 0.62 Sr 0.3 Al 2 Si 2 O 8 :0.08Eu 2+ , (Ca, Sr) AlSiN 3 :Eu 2+ and 365 nm NUV chips were successfully packaged into white LED devices. The colour rendering index (Ra) of the prepared white LED devices was 87, R9 was 89, the colour coordinates were (0.3763, 0.3382), and the colour temperature was 3759 K, which effectively solves the problem of the lack of cyan luminescent components in white LED devices and simplifies the manufacturing process of white LEDs.
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ANALYTICAL CHEMISTRY
·
2023
·
IF 7.4
Qiu-Yue Cheng,Ting Wang,Jun Hu,Hong-Yuan Chen,Jing-Juan Xu
Visible-light-mediated heterogeneous photocatalysis has recently emerged as an environmentally friendly and energy-sustainable alternative for organic transformations. Despite the advancements in developing wide varieties of photocatalysts during the past decades, the accurate probing and identification of the photogenerated species, especially the short-lived radical intermediates, are still challenging. In this work, we reported a hybrid ion emitter that integrated with a pico-liter heterogeneous photocatalytic reactor, which was fabricated by depositing the photocatalyst (e.g., TiO2) into the front tip of a quartz micropipette. Benefited from the dual-function feature of the hybrid micropipette (i.e., a clog-free tip-confined pico-liter reactor for heterogeneous photocatalysis and an ion emitter for nanoelectrospray ionization), sensitized photoredox reactions at the catalyst–solution interface can be triggered upon visible-light irradiation using a cheap LED laser (453 nm), and the newly produced transient radical intermediates can be rapidly transformed into gaseous ions for mass spectrometric identification. Using this novel low-delay coupling device, photogenerated intermediates, including the cationic radicals produced during the photooxidation of anilines and the anionic radicals produced during the photoreduction of quinones, were successfully captured by mass spectrometry. We believe that our hybrid photochemical microreactor/ion emitter has provided a new and powerful tool for exploring the complicated heterogeneous photochemical processes, especially their ultrafast initial transformations.
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Advanced Optical Materials
·
2023
·Vol. 11
·期 15
·2300218
·
IF 9
Shihui He,Shiqiang Hao,Liubing Fan,Kunjie Liu,Chuxin Cai,Christopher Wolverton,Jing Zhao,Quanlin Liu
Organic–inorganic metal halides (OIMHs) with high-efficiency solar spectrum-like emission are attracting broad and current interest. Here, five 0D Zn-based hybrid halides are synthesized based on aromatic organic cations with different carbon-chain lengths: C 6 H 5 CH 2 NH 3 + (PMA + ) and C 6 H 5 (CH 2 ) 4 NH 3 + (PBA + ). (PMA) 2 ZnCl 4 exhibits the highest photoluminescence quantum yield of 37.2% of reported Zn-based white-emission OIMHs. The emission spectrum of (PBA) 2 ZnI 4 indicates a color rendering index of 98, which is the highest among single-component white-light-emitting phosphors. Spectral characterizations and density functional theory calculations demonstrate that the extremely broad emission of (PBA) 2 ZnI 4 originates from the synergistic emission of organic cations and self-trapped excitons. The optical properties of the obtained (PMA) 2 ZnBr 4 , (PMA) 2 ZnI 4 ·H 2 O, and (PBA) 2 ZnCl 4 are also characterized for comparison, and with the same organic cations, the PLQY decreases from chloride to bromide to iodide. This work demonstrates that the selection of appropriate organics and halogens can enable fine tuning of single-component white-light emission, satisfying varying needs for solid-state lighting.
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LANGMUIR
·
2023
·
IF 3.9
Yingxiang He,Jianmin Gu,Adan Li
Gray bismuth chloride nanosheets with a highly enhanced electric field intensity were prepared by a simple and efficient method. Their energy gap is reduced to 2.35 eV. The prepared nanosheets show high photocatalytic activity for the degradation of rhodamine B under visible light. The resulting samples were characterized by X-ray diffractometry, high-resolution scanning electron microscopy, X-ray photoelectron spectroscopy, infrared spectroscopy, UV–vis diffuse reflectance spectroscopy, specific surface area analysis, electrochemical analysis, electron paramagnetic resonance, and UV–vis spectroscopy. The photocatalytic activity of prepared BiOCl was evaluated by the degradation of RhB. The prepared BiOCl sample (0.5 g/L) could completely degrade RhB (10 mg/L) within 10 min, and its visible photocatalytic activity was 80 times that of the original white BiOCl. Superoxide radicals were the main active substance involved in organic degradation.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Yan-Zi Wang,Xin-Li An,Xiao-Ting Fan,Qiang Pu,Hu Li,Wen-Zhen Liu,Zhuo Chen,Jian-Qiang Su
Inhibition of plasmid transfer, including transformation and conjugation, is essential to prevent the spread of plasmid-encoded antimicrobial resistance. Photosensitizers have been successfully used in the treatment of serious infectious diseases, however, the effects of photosensitizers on the plasmid transfer are still elusive. In this study, we determined the transformation and conjugation efficiency of plasmid pUC19 and pRP4, respectively, when exposed to a photosensitizer (Visible Light-activated Rose Bengal, VLRB). The results showed that the activation of VLRB resulted in up to a 580-fold decrease in the transformation frequency of pUC19 and a 10-fold decrease in the conjugation frequency of pRP4 compared with the non-VLRB control. The inhibition of pUC19 transformation by VLRB exhibited a dose-dependent manner and was attributed to the changes in the plasmid conformation. The inhibition of pRP4 conjugation was associated with the generation of extracellular free radicals , induced oxidative stress , suppression of the mating pair formation gene ( trbBp ) and DNA transfer and replication gene ( trfAp ), and enhanced expression of the global regulatory genes ( korA , korB , and trbA ). These findings highlight the potential of visible light-activated photosensitizer for mitigating the dissemination of plasmid-encoded antibiotic resistance genes.
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ENVIRONMENTAL TECHNOLOGY
·
2023
·
IF 2.8
Zhendong Wang,Zhexin Zhu,Gangqiang Wang,Xiaoji Ma,Wangyang Lu
Iron (II) phthalocyanine (FePc) is loaded on the surface of the tourmaline (TM) by the reflow method to obtain FePc/TM. This research effectively prevents the π-π stacking of FePc, increased the effective utilization rate of PMS activation under solar light, and further improved the catalytic performance of the catalytic system. The catalytic oxidation efficiency of FePc/TM on carbamazepine (CBZ) and sulfadiazine (SD) can reach 99% under solar light for 15 and 5 min, the total organic carbon (TOC) removal rate can reach 58% and 69% under solar light for 120 min. After 6 cycles, the CBZ removal rate remained above 95%. In addition, the FePc/TM catalytic system has an excellent removal rate for other pharmaceuticals. The results of spin-trapped electron paramagnetic resonance and classical quenching experiments show that FePc/TM can effectively activate PMS to generate active species under solar light, including superoxide radical (•O2−), singlet oxygen (1O2), hydroxyl radicals(•OH), and sulphate radicals (SO4•−). The intermediates of CBZ were identified by Ultra-high performance liquid chromatography and high resolution mass spectrometry, and the degradation pathway was proposed. As the reaction progresses, all CBZ and intermediates are reduced and converted into small acids, or mineralized to H2O, CO2. This work provides an alternative method for the design of efficient activation of PMS activation catalysts under solar light to eliminate residual pharmaceuticals in actual water bodies.
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