Latest ArticlesIn this work, we developed plasmonic photocatalyst composed of CuPd alloy nanoparticles supported on TiN, the optimized Cu3Pd2/TiN catalyst shows excellent conversion (> 96%) and selectivity (> 99%) for Heck reaction at 50 ℃ under visible light irradiation. By in-situ spectroscopic investigations, we find that visible light excitation could achieve stable metallic Cu species on the surface of CuPd alloy nanoparticles, thereby eliminating the inevitable surface oxides of Cu based catalyst. The in-situ formed metallic Cu species under irradiation take advantage of the strong interactions of Cu with visible light, and manifest in the localized surface plasmon resonances (LSPR) photoexcitation. Visible light excitation could further promote the charge transfer between catalytic Pd component and the support TiN, resulting in electron-rich Pd sites on CuPd/TiN. Moreover, light excitation on CuPd/TiN generates strong chemisorption of iodobenzene and styrene, favoring the activation of reactants for Heck reaction. DFT calculations suggest that electron-rich CuPd sites ideally lower the activation energy barrier for the coupling reaction. This work provides valuable insights for mechanistic understanding of plasmonic photocatalysis.
Photocatalytic technology harnesses solar energy to facilitate chemical transformations, presenting significant potential in energy generation and environmental remediation. However, the conventional O2 evolution process is hindered by high reaction barriers and inefficiencies, which limit its widespread application. Therefore, exploring novel photocatalytic coupling strategies to replace water oxidation has become a key route to enhance the efficiency of H2 production. In this review, organic pollutants removal and the valorization of organics as substitutes for water oxidation coupling strategies for photocatalytic H2 production are comprehensively summarized. These strategies not only circumvent the high reaction barriers associated with O2 evolution to enhance the H2 production but also aid in the removing of organic pollutants or synthesis of value-added chemicals. We also present future research directions and underscore the significance of advanced catalyst design, in-depth analysis of reaction mechanisms, and systematic optimization strategies in realizing an efficient and sustainable photocatalytic process. This guidance is anticipated to provide theoretical and practical new insights for the future development of photocatalytic coupling reactions, fostering further explorations in the realm of renewable energy and environmental governance.
The high conductivity of electrocatalyst can eliminate the Schottky energy barrier at the interface of heterogeneous phases during an electrocatalytic reaction and accelerate the rapid electron transfer to the catalytic active center. Therefore, the electronic conductivity is a vital parameter for oxygen reduction reaction (ORR). Covalent triazine frameworks (CTFs) have shown great potential application as electrocatalysts in ORR with a merit of the diverse building blocks. However, the intrinsic low conductivity and high impedance of CTFs could be significant setbacks in electrocatalytic application. Herein, CTFs were constructed by introducing F and N co-modification for efficient 2e− ORR. Compared with the pristine CTF, the co-presence of F, N could increase the conductivity obviously by 1000-fold. As a result, F-N-CTF exhibits enhanced catalytic performance of H2O2 generation and selectivity towards reaction pathways. This work reveals the importance of conductivity optimization for CTFs and provides guidance for designing high conductivity non-metallic organic semiconductor catalysts for 2e− ORR.
The synthesis of polyurethanes (PUs) from the reaction of low molecular weight poly(ethylene carbonate) diol (PECD) is rarely investigated. This work reports a novel PU with excellent mechanical properties from the solution polymerization of 4,4′-diphenylmethane diisocyanate (MDI) with PECD that was derived from the copolymerization of carbon dioxide (CO2) and ethylene oxide (EO). The tensile strength, the elongation at break and 300% constant tensile strength of the PECD-PU were up to 66 ± 2 MPa, 880% ± 50% and 13 MPa, respectively, higher than the control PUs from the reaction of MDI with commercial polyethers or polyesters. The PECD-PU with high CO2 carbonate content exhibited good solvent resistance and chemical stability. Of importance, the mechanical properties and chemical resistance of PECD-PU were significantly enhanced with the increasing content of CO2, i.e., the carbonate unit in PECD. This work provides comprehensive properties of PECD-derived PUs, indicating that PECD is a competitive precursor for the preparation of PU and has broad application prospects.
Benzotriazole (BTA)-based A2-A1-D-A1-A2 type wide-bandgap (WBG) non-fullerene acceptors (NFAs) have shown promising potential in indoor photovoltaic, and in-depth investigation of their structure-property relationship is of great significance. Herein, we explored the chlorination effect of the side chain on the terminals. We introduced Cl atoms into the benzyl side chains in parent BTA5 to synthesize two NFAs, BTA5-Cl with mono-chlorinated benzyl groups and BTA5-2Cl containing bi-chlorinated benzyl groups. We chose D18-Cl with deep-energy levels and strong crystallinity to pair with these three acceptors, affording high photovoltage and photocurrent. With the stepwise chlorination, the open-circuit voltage (VOC) values decrease from 1.28, 1.22, to 1.20 V, while the corresponding power conversion efficiencies (PCEs) improve from 5.07%, 9.15%, to 10.96%. Compared with BTA5-based OSCs, introducing Cl atoms downshifts the energy levels and slightly increases the non-radiative energy loss (0.14 < 0.17 < 0.19 eV), resulting in a sequential decrease in VOC. However, more chlorine atom replacements produce more effective exciton dissociation, higher charge transfer, and balanced carrier mobility in the blend films, ultimately achieving better PCEs. This work indicates that chlorination of the benzyl group on the terminals can improve the device's performance, implying good application potential in indoor photovoltaics.
Disulfidptosis, a novel mechanism of programmed cell death through the disruption of tumor metabolic symbiosis (TMS), has showed tremendous potential in cancer therapy. However, the efficacy of disulfidptosis is limited by poor permeability of drugs in solid tumors. Herein, hydrogen sulfide (H2S) and near-infrared (NIR) light-driven nanomotors (denoted as HGPP) have been constructed to efficiently penetrate tumors and induce disulfidptosis. HGPP demonstrate glutathione (GSH)-responsive release of H2S, which combined with NIR light-induced photothermal effect drive HGPP movement to facilitate deep tumor penetration. The released H2S induces tumor acidosis and disrupts TMS, where disulfide accumulation following cell starvation leads to disulfidptosis. In addition, HGPP induce hepatoma specific cellular uptake and catalyze the conversion of glucose and oxygen to produce hydrogen peroxide (H2O2), leading to glucose starvation. Overall, this study has developed a multifunctional Janus nanomotor that provides a novel strategy for disulfidptosis-based solid tumor therapy.
Photocatalytic overall pure water splitting is a promising method for generating green hydrogen energy under mild conditions. However, this process is often hindered by sluggish electron-hole separation and transport. To address this, a step-scheme (S-scheme) B-doped N-deficient C3N4/O-doped C3N5 (BN-C3N4/O-C3N5) heterojunction with interfacial B-O bonds has been constructed. Utilizing Pt and Co(OH)2 as co-catalysts, BN-C3N4/O-C3N5 S-scheme heterojunction demonstrates significantly enhanced photocatalytic activity for overall pure water splitting under visible light, achieving H2 and O2 evolution rates of 40.12 and 19.62 µmol/h, respectively. Systematic characterizations and experiments revealed the performance-enhancing effects of the enhanced built-in electric field and the interfacial B-O bonding. Firstly, the strengthened built-in electric field provides sufficient force for rapid interfacial electron transport. Secondly, by reducing the transport energy barrier and transfer distance, the interfacial B-O bonds facilitate rapid recombination of electrons and holes with relatively low redox potential via the S-scheme charge-transfer route, leaving the high-potential electrons and holes available for H+ reduction and OH− oxidation reactions. Overall, the photocatalytic efficiency of BN-C3N4/O-C3N5 S-scheme heterojunction was significantly improved, making it a promising approach for green hydrogen production through overall pure water splitting.
As battery technology evolves and demand for efficient energy storage solutions, aqueous zinc ion batteries (AZIBs) have garnered significant attention due to their safety and environmental benefits. However, the stability of cathode materials under high-voltage conditions remains a critical challenge in improving its energy density. This review systematically explores the failure mechanisms of high-voltage cathode materials in AZIBs, including hydrogen evolution reaction, phase transformation and dissolution phenomena. To address these challenges, we propose a range of advanced strategies aimed at improving the stability of cathode materials. These strategies include surface coating and doping techniques designed to fortify the surface properties and structure integrity of the cathode materials under high-voltage conditions. Additionally, we emphasize the importance of designing antioxidant electrolytes, with a focus on understanding and optimizing electrolyte decomposition mechanisms. The review also highlights the significance of modifying conductive agents and employing innovative separators to further enhance the stability of AZIBs. By integrating these cutting-edge approaches, this review anticipates substantial advancements in the stability of high-voltage cathode materials, paving the way for the broader application and development of AZIBs in energy storage.
Highly toxic phosgene, diethyl chlorophosphate (DCP) and volatile acyl chlorides endanger our life and public security. To achieve facile sensing and discrimination of multiple target analytes, herein, we presented a single fluorescent probe (BDP-CHD) for high-throughput screening of phosgene, DCP and volatile acyl chlorides. The probe underwent a covalent cascade reaction with phosgene to form boron dipyrromethene (BODIPY) with bright green fluorescence. By contrast, DCP, diphosgene and acyl chlorides can covalently assembled with the probe, giving rise to strong blue fluorescence. The probe has demonstrated high-throughput detection capability, high sensitivity, fast response (within 3 s) and parts per trillion (ppt) level detection limit. Furthermore, a portable platform based on BDP-CHD was constructed, which has achieved high-throughput discrimination of 16 analytes through linear discriminant analysis (LDA). Moreover, a smartphone adaptable RGB recognition pattern was established for the quantitative detection of multi-analytes. Therefore, this portable fluorescence sensing platform can serve as a versatile tool for rapid and high-throughput detection of toxic phosgene, DCP and volatile acyl chlorides. The proposed "one for more" strategy simplifies multi-target discrimination procedures and holds great promise for various sensing applications.
Copper (Cu) is widely used in the electrochemical carbon dioxide reduction reaction (ECO2RR) for efficient methane (CH4) product. However, the morphology and valence of Cu-based catalysts are usually unstable under reaction conditions. In this work, we prepared Ce-doped MOF-199 precursor (Ce/HKUST-1) and further obtained nanoparticle electrocatalyst Ce/CuOx-NPs by cyclic voltammetry (CV) pretreatment. The Faradic efficiency of methane () maintains above 62% within a broad potential window of 350 mV and the maximum reaches 67.4% with a partial current density of 293 mA/cm2 at −1.6 V vs. a reversible hydrogen electrode. Catalyst characterization and theoretical calculations revealed that the unique electronic structure and large ionic radius of Cerium (Ce) not only promoted the generation of key intermediate *CO but also lowered energy barrier of the *CO to *CHO step. This study provides a novel and efficient catalyst for methane production in ECO2RR and offers profound insights into constructing high performance Cu-based catalysts.
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