The selective conversion of 5-hydroxymethylfurfural (HMF) is crucial for biomass valorization, yet its complex pathways challenge precise product control. Herein, we report a tannic acid (TA)-mediated bifunctional TA@Cu2O-Cu catalyst that enables the on-demand electroreduction of HMF to 2,5-dihydroxymethylfuran (DHMF) or electrooxidation to 2,5-furandicarboxylic acid (FDCA). For HMF reduction, the catalyst achieves 99% Faradaic efficiency (FE) and a DHMF production rate of 140 μmol cm-2 h-1 (flow cell: 730 μmol cm-2 h-1), vastly surpassing unmodified Cu NPs (51%, 30 μmol cm-2 h-1). Notably, stable operation for 200h in a membrane electrode assembly (MEA) electrolyzer enables gram-scale DHMF synthesis (21.5g). For HMF oxidation, it also delivers 99% FE toward FDCA, with a 1.7-fold faster production rate than unmodified Cu NPs. In-situ spectroscopic and density functional theory (DFT) calculations corroborate that TA endows the catalyst with favored HMF adsorption thermodynamics. Owing to the electronic modulation effect of TA, it stabilizes Cu+/Cu0 to accelerate HMF reduction and simultaneously facilitates CuOOH formation to lower the oxidation reaction barrier. Furthermore, a bifunctional light-driven paired electrolysis system co-generates DHMF and FDCA at 24.3 and 7.3mgh-1, respectively, under AM 1.5G illumination. This ligand-induced charge modulation strategy offers new insights into biomass valorization catalyst design.

Accurate detection of alpha-fetoprotein (AFP) is vital for early cancer diagnosis, yet traditional immunoassays suffer from limited sensitivity. Although surface-enhanced Raman scattering (SERS) is a formidable analytical tool, existing platforms often encounter a performance saturation bottleneck upon reaching equilibrium, lacking a controllable regulation mechanism capable of guiding the stepwise intensification of hotspots for continuous gain throughout the analytical process. This work proposes a metal-ion-mediated cyclic amplification strategy. Inspired by coordination chemistry, aluminum ions (Al3+) serve as highly specific "molecular glues" that coordinate with the surface ligands of His/4-MBA-functionalized gold nanoparticles (His/4-MBA@Au NPs) to trigger their controlled aggregation. By iteratively introducing these Al3+ ions and functionalized Au NPs onto a solid-phase immunocomplex, we achieved a stepwise, programmable densification of 3D SERS hotspots. Unlike conventional "single-trigger" modes, this multicycle process allows for the evolutionary growth of assay performance, where hotspot tunability is realized by adjusting the number of cycles: initial stages (Cycle 1) provide a broad dynamic range, while highly densified hotspot architectures (Cycle 5) deliver superior ultratrace sensitivity. Consequently, the limit of detection (LOD) for the target AFP improved progressively from 8.6 pg·mL-1 in Cycle 1 down to an ultimate 0.043 pg·mL-1 in Cycle 5. This strategy exhibits excellent anti-interference capability in human serum, offering a versatile blueprint for ultratrace biomarker detection.

Triazine herbicides are widely detected in food and pose significant hazards to ecosystems and human health. In this study, a nanoconfined composite of task-specific ionic liquids (TSILs) within hollow porous carbon spheres (HPCS), denoted TSILs@HPCS, was synthesized via post-impregnation for selective enrichment and efficient extraction of triazine herbicides. Hydrophobic TSILs incorporating [NTf2-] anion were systematically prepared. Confinement within HPCS tunable pores yielded a 6.0-fold increase in triazine herbicide adsorption capacity relative to pristine HPCS. The TSILs@HPCS composite serves as a multifunctional adsorbent, enabling the simultaneous sorptive removal, highly sensitive detection, and sieving of analytes. A dispersive solid-phase extraction method coupled with high-performance liquid chromatography was developed to quantify trace triazine herbicides in complex food matrices. This approach demonstrated low detection limits (0.06-0.12 μg kg-1) and high enrichment factors (124-192), confirming its suitability for residue analysis. These results establish TSILs@HPCS as a promising adsorbent for preconcentrating triazine herbicides in food samples.

The electrochemical nitrogen oxidation reaction (NOR) provides a method for converting N-2 and H2O into nitrate with zero CO2 emissions, offering an alternative to the energy-intensive Haber-Bosch and Ostwald processes. This study investigates the electrosynthesis of nitrate using air-saturated electrolyte, inspired by natural nitrogen fixation during thunderstorms. By employing Pd2+ and S2--doped SnO2 nanoparticles on n-butyl triethyl ammonium bromide-functionalized polypyrrole/graphene oxide (Pd/S-SnO2@BTAB/PPy/GO), improvements in nitrate yield and Faradaic efficiency are achieved at a potential of 1.77 V vs reversible hydrogen electrode in air-saturated electrolyte, compared to the NOR performance in a N-2-saturated electrolyte. Characterization confirms that Pd sites serve as catalytic centers for NOR, with isotope labeling experiments revealing that the N element in the produced nitrate originated entirely from N-2 gas, while the excess O-2 involved in the reaction contributes to the partial oxygen content of the generated nitrate. Theoretical calculations propose a reaction pathway wherein O-2 is first adsorbed onto the electrocatalyst before reacting with N-2. Although intermediates like NO and N2O can form in air-saturated electrolyte, they still require an electrocatalyst for conversion to nitrate. The NOR process in the air-saturated electrolyte includes the traditional 10-electron NOR process as well as additional 8-electron, 6-electron, and 2-electron NOR processes. This research clarifies the role of O-2 in nitrate electrosynthesis and presents a pathway for nitrate production, aligning with environmental objectives and addressing current energy challenges.

In situ growth of co-catalysts on BiVO4 (BVO) to enhance photoelectrochemical (PEC) water splitting performance has been extensively reported. However, the understanding of the synergistic effects among various elements, especially at the interface between the semiconductor and cocatalyst, has received insufficient attention. In this study, we report a Co, Ni and Mn trimetallic fluoride-modified BVO photoanode featuring a unique interfacial chemical bond (V-F). Under AM 1.5 G illumination, an exciting photocurrent density of 6.05 mA cm-2 was achieved at 1.23 V vs. RHE by the integrated BVO/CoNi0.18Mn0.12(OH)xF photoanode and over 98% of the initial photocurrent was maintained after 10 h of photoelectrolysis. Control experiments and theoretical calculations demonstrate that the V-F interfacial bond stabilizes the Co2+active sites. It serves as a transmission gear, interlinking the migration of interfacial charge and the regeneration of cocatalyst, endowing the photoanode with significant activity and stability. Furthermore, we have systematically elucidated the role of the individual Co, Ni, and Mn components in the synergistic cocatalyst layer. The interfacial modification provides novel insights into developing advanced photoanodes towards PEC water splitting. (c) 2025, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.

To overcome the limitations of high energy consumption and low selectivity in conventional antibiotic treatment methods, this study developed a sodium percarbonate (SPC)-activated piezoelectric-photocatalytic system using a nitrogen-doped carbon quantum dot/molybdenum disulfide (N-CQDs/MoS2) composite to degrade oxytetracycline (OTC). The catalyst was synthesized via a hydrothermal method and characterized by X-ray diffraction (XRD), scanning electron microscopy with energy-dispersive X-ray spectroscopy (SEM-EDS), piezoresponse force microscopy (PFM), and electrochemical analysis. Results showed that nitrogen-doped carbon quantum dots significantly enhanced the piezoelectric and photocatalytic performance of MoS2. Reaction conditions were optimized using response surface methodology (RSM), determining the optimal parameters as OTC concentration of 10.68 mg/L, catalyst dosage of 0.46 g/L, and SPC dosage of 0.21 g/L. Under these conditions, a degradation efficiency of 99.52 % was achieved within 25 min, closely matching the experimental result of 99.18 %. The degradation kinetics followed a quasi-first-order model (k = 0.0752 min-1), confirming the model's reliability. Radical scavenging experiments and electron paramagnetic resonance (EPR) analysis identified h+, center dot OH, and O2 center dot as the main reactive species. Ecotoxicity assessment showed low toxicity of the degradation products, indicating good environmental safety. The catalyst maintained a high degradation efficiency of 96 % after five cycles, demonstrating excellent stability and reusability.

To address the increasing global challenges of energy shortages and water pollution caused by organic contaminants, developing efficient and sustainable water treatment technologies has become a key focus in environmental science research. Recently, photoactivated sodium percarbonate (SPC) has gained attention in advanced oxidation processes for degrading organic pollutants due to its high reactivity, environmental compatibility, and ease of storage and handling. This review systematically summarizes recent advances and engineering application potential of photoactivated SPC systems for removing organic pollutants, based on nearly one hundred relevant studies. First, the paper analyzes the UV/SPC system in detail, focusing on the generation of reactive oxygen species (ROS) under different light sources (e.g., ultraviolet and visible light) and their roles in organic pollutant degradation pathways. Second, focusing on reaction condition optimization, this review evaluates how key parameters—SPC dosage, solution pH, coexisting inorganic ions, and natural organic matter—affect pollutant degradation efficiency and reaction selectivity. Furthermore, a comparative analysis examines SPC system performance in degrading typical organic pollutants such as dyes, pesticides, and endocrine-disrupting chemicals. In addition, the review assesses the UV/SPC system’s ecological toxicity and economic feasibility. The established "mechanism-performance-sustainability" evaluation framework will bridge the knowledge gap between researchers and engineers.

Selective electrocatalytic semi-hydrogenation (ECSH) of alkynes in water using Cu catalysts is highly relevant for the production of value-added chemicals. However, achieving high olefin selectivity still poses extreme challenges due to the susceptibility of the copper cathode in a reduction environment. Herein, a small molecule modulation electrodeposition strategy is introduced that regulates the structure of Cu-based materials through modification with citric acid (CA) ligands, aiming for highly active and selective ECSH. The as-prepared EDCu-CA electrode achieves more than 97% alkyne conversion and 99% olefin selectivity. In-situ Raman and Auger electron spectroscopy (AES) data provide evidence that active Cu+ sites can stably exist in the EDCu-CA during the catalytic process. Density functional theory (DFT) calculations indicate that the modulation by CA contributes to maintaining Cu in a positive valence state, and Cu+ can inhibit the over-hydrogenation of olefins. Moreover, by utilizing a large-area electrode for long-term electrolysis, g-level conversion and a 92% separation yield of olefin can be achieved, demonstrating a viable application prospect. This study offers a promising route for designing Cu-based catalysts for the highly selective electrocatalytic conversion of organic substrates to value-added chemicals in water.

Unbiased photoelectrochemical (PEC) H 2 O 2 production offers a sustainable alternative to the energy‐intensive anthraquinone process, yet faces critical bottlenecks: inefficient charge separation, uncontrolled two‐electron oxygen reduction reaction (2e − ORR) pathways, and high‐purity O 2 requirements. Herein, we report an efficient unbiased PEC system for H 2 O 2 production under ambient air. The key innovation involves the strategic implementation of boron nitride (BN) serves a dual role as a charge transfer mediator and ORR pathway modulator. At the photoanode, BN functions as a hole‐extraction layer, because of elevating the valence band position of BiVO 4 (BVO), effectively suppressing interfacial charge recombination between the BVO photoanode and the FeNiOOH cocatalyst, resulting in a photocurrent density achieving 6.08 mA cm −2 at 1.23 V RHE . At the cathode, BN acts as a “reaction helmsman”, tuning the binding energy of the *OOH intermediate and enabling the CoPc + BN to achieve 97% 2e − ORR selectivity at −0.3 V Ag/AgCl . As a result, the integrated system delivers a sustained H 2 O 2 production rate of 1.22 ± 0.14 mM cm −2 h −1 over 16 consecutive cycles. This study provides an innovative solution to address the key challenges in bias‐free H 2 O 2 production.

Unbiased photoelectrochemical (PEC) H 2 O 2 production offers a sustainable alternative to the energy-intensive anthraquinone process, yet faces critical bottlenecks: inefficient charge separation, uncontrolled two-electron oxygen reduction reaction (2e − ORR) pathways, and high-purity O 2 requirements. Herein, we report an efficient unbiased PEC system for H 2 O 2 production under ambient air. The key innovation involves the strategic implementation of boron nitride (BN) serves a dual role as a charge transfer mediator and ORR pathway modulator. At the photoanode, BN functions as a hole-extraction layer, because of elevating the valence band position of BiVO 4 (BVO), effectively suppressing interfacial charge recombination between the BVO photoanode and the FeNiOOH cocatalyst, resulting in a photocurrent density achieving 6.08 mA cm −2 at 1.23 V RHE . At the cathode, BN acts as a “reaction helmsman”, tuning the binding energy of the *OOH intermediate and enabling the CoPc + BN to achieve 97% 2e − ORR selectivity at −0.3 V Ag/AgCl . As a result, the integrated system delivers a sustained H 2 O 2 production rate of 1.22 ± 0.14 mM cm −2  h −1 over 16 consecutive cycles. This study provides an innovative solution to address the key challenges in bias-free H 2 O 2 production.

In recent years, the efficient removal of organic pollutants from wastewater has emerged as a critical area of global research interest. Against this backdrop, an array of innovative technologies for wastewater treatment has been developed. Among numerous advanced oxidation processes (AOPs), periodate (PI), an emerging oxidizing agent in AOPs, has garnered significant attention from researchers. Particularly, the integration of ultrasound (US)-activated PI systems has been recognized as an exceptionally promising approach for the synergistic degradation of organic pollutants in wastewater. In this paper, we conducted a thorough analysis of the mechanisms underlying the degradation of organic pollutants using the US/PI system. Furthermore, we comprehensively delineated the effects of ultrasonic power, periodate concentration, temperature, pH, coexisting inorganic ions, and dissolved organic matter on the removal efficiency of organic pollutants and summarized application cases of the US/PI system for the degradation of different pollutants. Finally, we also offered prospective discussions on the future trajectories of US/PI technology development.

In recent decades, water pollution caused by emerging contaminants such as pharmaceuticals, has attracted much attention. Antibiotics are commonly used pharmaceuticals, and their residue in water may accelerate the development of antibiotic resistance genes, which can produce resistance to the treatment of diseases. In this study, two energy-based systems, heat/peroxymonosulfate (PMS) and ultrasound (US)/PMS were chosen to treat the typical antibiotic tetracycline (TC) in water. The influencing factors and kinetic equations of TC degradation by heat/PMS and US/PMS were investigated and the rates of TC degradation by the two systems were compared. The results showed that the optimal PMS concentration required for TC degradation in both systems was 0.3 mM, and neither system was affected by solution pH. The power of the US in the US/PMS system was as important as the temperature in the heat/PMS system because they provided activation energy. Both heat and US could activate PMS to degrade TC, and US was slightly superior with 80% TC removal under the conditions of [TC] = 20 mg/L, [PMS] = 0.3 mM, pH = 6.4, T = 20 °C, and US power = 550 W. US is considered to be more advantageous in activating PMS to degrade TC.

Inverted perovskite solar cells are promising candidates in photovoltaic fields due to their low-temperature processing, simplified fabrication, and enhanced stability when compared with the conventional configuration. However, the significant non-radiative recombination losses and energy alignment mismatch at the perovskite/C 60 interface limit the device 's performance and long-term stability. To overcome this drawback, we introduced trifluoromethoxy-functionalized phenethylammonium iodide salts with high polarity between the perovskite and C 60 electron transporting layer. This bifunctional interlayer not only effectively passivates the perovskite surface and interface but also reduces the minority carriers through the band rearrangement at this interface, thus significantly suppressing the deteriorating interfacial non-radiative recombination. The modified interlayer also facilitates electron extraction by reducing the offset between the perovskite and C 60 , contributing to an improved photocurrent and fill factor. The resultant inverted perovskite solar cell based on a Cs 0.05 FA 0.85 MA 0.10 Pb(I 0.95 Br 0.05 ) 3 composition reveals a power conversion efficiency of 24.7 % at the reverse scan and shows negligible efficiency loss after 600 h of maximum power point tracking under one -sun illumination. Overall, this feasible deposition of ammonium -based interlayer establishes a successful demonstration of efficient and stable inverted devices to accelerate the commercialization of perovskite photovoltaics.

Transition metal chalcogenides (TMCs) are widely used in photocatalytic fields such as hydrogen evolution, nitrogen fixation, and pollutant degradation due to their suitable bandgaps, tunable electronic and optical properties, and strong reducing ability. The unique 2D malleability structure provides a pre-designed platform for customizable structures. The introduction of vacancy engineering makes up for the shortcomings of photocorrosion and limited light response and provides the greatest support for TMCs in terms of kinetics and thermodynamics in photocatalysis. This work reviews the effect of vacancy engineering on photocatalytic performance based on 2D semiconductor TMCs. The characteristics of vacancy introduction strategies are summarized, and the development of photocatalysis of vacancy engineering TMCs materials in energy conversion, degradation, and biological applications is reviewed. The contribution of vacancies in the optical range and charge transfer kinetics is also discussed from the perspective of structure manipulation. Vacancy engineering not only controls and optimizes the structure of the TMCs, but also improves the optical properties, charge transfer, and surface properties. The synergies between TMCs vacancy engineering and atomic doping, other vacancies, and heterojunction composite techniques are discussed in detail, followed by a summary of current trends and potential for expansion. In this work, the vacancy engineering of 2D transition metal chalcogenides (TMCs) is reviewed from two aspects: introduction strategy and application in photocatalysis. Subsequently, the photocatalytic process of 2D TMCs with vacancy engineering is introduced. The synergies between vacancy engineering and TMCs modified by other strategies are discussed. Finally, expectations and suggestions for the development of transition metal chalcogenides are presented. image

As the contamination and enrichment in food chain of levofloxacin (LV) antibiotics have caused a significant threat to life safety, the instant detection of LV has become an urgent need. Here, a PDI-functionalized imine-based covalent organic framework (PDI-COF300) was prepared by the electrostatic self-assembly method as fluorescent probe for smartphone visual detection of LV, which exhibited excellent fluorescence quantum yield (82.68%), greater stability, high sensitivity with detection limit of 0.303 μM. Based on the results of molecular docking and Stern-Volmer equation, the LV detection by PDI-COF300 was mainly a static quenching process through π-π stacked hydrophobic interactions and fluorescence resonance energy transfer. Besides, PDI-COF300 was applied to LV detection in environmental medium and milk samples with recoveries from 85.56% to 108.34% and relative standard deviations <2.70%. This work also provided a new general strategy for using PDI-COF in smartphone devices and fluorescent papers for LV fluorescence detection and microanalysis.

A heterogeneous Co4O4-poly cocatalyst demonstrated superior catalytic performance in water oxidation.

Regulating the interfacial charge transfer behavior between cocatalysts and semiconductors remains a critical challenge for attaining efficient photoelectrochemical water oxidation reactions. Herein, using bismuth vanadate (BiVO4 ) photoanode as a model, it introduces an Au binding bridge as holes transfer channels onto the surfaces of BiVO4 , and the cyano-functionalized cobalt cubane (Co4 O4 ) molecules are preferentially immobilized on the Au bridge due to the strong adsorption of cyano groups with Au nanoparticles. This orchestrated arrangement facilitates the seamless transfer of photogenerated holes from BiVO4 to Co4 O4 molecules, forming an orderly charge transfer pathway connecting the light-absorbing layer to reactive sites. An exciting photocurrent density of 5.06 mA cm-2 at 1.23 V versus the reversible hydrogen electrode (3.4 times that of BiVO4 ) is obtained by the Co4 O4 @Au(A)/BiVO4 photoanode, where the surface charge recombination is almost completely suppressed accompanied by a surface charge transfer efficiency over 95%. This work represents a promising strategy for accelerating interfacial charge transfer and achieving efficient photoelectrochemical water oxidation reaction.

Energy scarcity and environmental pollution concerns have become substantial impediments to sustainable global economic development. The advent of semiconductor photocatalysis technology provides a potential possibility for effectively alleviating excessive energy consumption and maintaining the long-term stability of the aqueous ecosystem. However, the inefficient transmission efficiency of charge carriers and the high recombination rate of photogenerated electron-hole pairs will culminate in the mediocre catalytic performance observed in conventional semiconductor materials. Fortunately, the piezo-photocatalysis ingeniously integrates the piezoelectric properties of piezoelectric crystals with the optoelectronic properties of semiconductors, thus building a theoretical system of photo-electric-chemical three-phase coupled catalysis. Currently, the photo-mechanical energy synergistic catalytic oxidation degradation process, as a cutting-edge technology based on clean renewable energy, has been perceived as a promising environmental remediation strategy. Herein, a critical review of the application of piezo-photocatalysis in environmental pollution control was delivered. We undertook a comprehensive analysis to elucidate the underlying enhancement mechanism of the piezoelectric effect on photocatalysis in terms of charge migration dynamics and pertinent energy band bending phenomena. In addition, we meticulously summarized diverse innovative methods for introducing vibration energy in piezo-photocatalytic degradation systems (ultrasound, fluid mechanical energy, airflow, self-assembled reactors, etc.). Then, state-of-the-art research advances in the field of environmental pollution control and the corresponding environmental decontamination mechanisms were elaborated based on various integration modes of catalysts (single component, noble metal deposition, heterojunction, coupled substrate materials, etc.). Eventually, an in-depth assessment of current limitations and development trends of piezo-photocatalytic degradation technology has been proposed, along with proactive strategies aimed at surmounting the existing challenges.

Due to the excellent properties of various carbon and carbon doped materials, they have served as activators in advanced oxidation processes. Initially, carbon and carbon doped materials were used to activate peroxymonosulfate or peroxydisulfate to remove organics in water. Recently, they have been employed to activate periodate to degrade recalcitrant organics. Activated carbon, biochar, modified biochar, graphene, and other different carbon doped materials have shown superb activation performance in activating periodate and are receiving more and more attention. However, no review related to carbon and carbon doped materials/periodate processes has been found. Therefore, this review mainly focuses on discussing the mechanism, effectiveness, and influencing factors of periodate activation toward recalcitrant organics via various carbon and carbon doped materials. Furthermore, the activation methods of periodate and the recognization of the active species generated in the reaction are also summarized. Finally, the obstacles encountered by carbon and carbon doped materials/periodate systems are also elaborated with considerable solutions. This review offers a profile for greater exploring carbon and carbon doped materials/periodate systems in decomposing recalcitrant organics and proposes future research ideas about periodate-based advanced oxidation.

Monoclinic BiVO4 is one of the most promising photoanode materials for solar water splitting. The photoelectrochemical performance of a BiVO4 photoanode could be significantly influenced by the noncovalent interactions of redox-inert metal cations at the photoanode-electrolyte interfaces, but this point has not been well investigated. In this work, we studied the Cs+-dependent surface reconstruction and passivation of BiVO4 photoanodes. Owing to the "structure breaker" nature of Cs+, the Cs+ at the BiVO4 photoanode-electrolyte interfaces participated in BiVO4 surface photocorrosion to form a Cs+-doped bismuth vanadium oxide amorphous thin layer, which inhibited the continuous photocorrosion of BiVO4 and promoted surface charge transfer and water oxidation. The resulting cocatalyst-free BiVO4 photoanodes achieved 3.3 mA cm-2 photocurrent for water oxidation. With the modification of FeOOH catalysts, the photocurrent at 1.23 VRHE reached 5.1 mA cm-2, and a steady photocurrent of 3.0 mA cm-2 at 0.8 VRHE was maintained for 30 h. This work provides new insights into the understanding of Cs+ chemistry and the effects of redox-inert cations at the electrode-electrolyte interfaces.