Xu Sun

Electrocatalytic hydrogen production is pivotal for advancing the transition to green energy. However, its widespread application is hindered by the limited efficiency of electrocatalysts and the sluggish kinetics of the anodic oxygen evolution reaction (OER). Developing high‐performance, durable, and cost‐effective electrocatalysts, coupled with the substitution of OER with thermodynamically more favorable oxidation reactions, represents a promising strategy to address these challenges. Herein, we successfully fabricated a novel transition metal‐based high‐entropy hydroxyl carbonate (HE‐HC) catalyst. Comprehensive experimental and computational characterizations demonstrate that the resulting catalyst exhibits superior catalytic activity for the benzyl alcohol oxidation reaction (BOR), achieving high selectivity and Faradaic efficiency (FE) toward the value‐added product, benzoic acid. This work not only presents a novel metal‐organic framework (MOF)‐derived high‐entropy catalyst for efficient alcohol oxidation co‐electrolysis but also provides fundamental insights into the design principles of multi‐metallic catalysts for coupled energy conversion and chemical synthesis processes.

Electrochemical CO₂ reduction reaction (CO₂RR) to formate presents a technoeconomic route for CO₂ utilization under mild conditions, yet practical implementation is constrained by the high energy consumption (>90% of total input) of the anodic oxygen evolution reaction (OER). Replacement of OER by partial methanol oxidation reaction (MOR) could lead to simultaneous formate production at both electrodes and remarkably reduce the overall energy consumption. Herein, we designed a two-electrode system featuring a nickel foam-supported crystalline/amorphous bismuth-bismuth nickel oxide composite cathode (Bi-BiNiO_x/NF) and a β-Ni(OH)₂ anode, achieving excellent formate production behavior. The crystalline/amorphous Bi-BiNiO_x/NF cathode delivers exceptional CO₂RR performance, achieving 98.9% formate Faradaic efficiency (FE_formate) at -0.90 V vs. RHE and maintaining >90.7% FE_formate over 72 h continuous operation—attributed to its Bi-Ni bimetallic synergy and crystalline/amorphous heterostructure that enhance active site exposure and reaction kinetics. The integrated CO₂RR||MOR system operates stably for 90 h at 2.2 V and 10 mA cm^-2, sustaining >90% FE_formate at both electrodes with a cell voltage (1.760 V) significantly lower than conventional CO₂RR||OER systems (1.953 V). This work demonstrates efficient concurrent formate electrosynthesis and establishes an energy-efficient paradigm for electrocatalytic CO₂ valorization through synergistic catalyst design and reaction pathway integration.

With the prevalence of electrochemiluminescence (ECL) in bioanalysis and clinical diagnostics, the development of efficient low-potential ECL systems has emerged as a research focus. Herein, a novel coreactant acceleration approach was reported based on FeNi layered double hydroxide enriched with oxygen vacancies (FeNi-LDH-V_O). The system produced notably strong ECL signals at -0.8 V when integrated with a Zr-porphyrin metal-organic framework (Zr-MOF). Mechanistic investigations revealed that the V_O in the FeNi-LDH provided abundant active sites that facilitated peroxydisulfate (S₂O₈^2-) adsorption and activation, which triggers the generation of highly reactive sulfate (SO₄^•-) and hydroxyl (^•OH) radicals. Efficient radical production played a key role in enhancing ECL output. Based on this mechanism, an ECL imaging biosensor was designed for visually detecting diazinon (DZN). In the presence of Mg²⁺, the DNAzyme catalyzed the site-specific cleavage of the ferrocene (Fc)-labeled strand, resulting in the release of Fc quenchers from the electrode surface and an ECL signal that is enhanced in a concentration-dependent manner. The biosensor exhibited a wide linear range (0.1 to 5.0 × 10³ nM), a low detection limit (7.6 pM), and excellent specificity and repeatability, showing potential for food marker detection.

An innovative dual-channel microfluidic photoelectrochemical (PEC) immunosensor was constructed for simultaneous determination of carbohydrate antigen 15-3 (CA15-3) and cancer antigen 125 (CA125). Herein, AgBr-sensitized La-doped BiOBr with surface oxygen vacancies (AgBr/La-BiOBr-OV) was synthesized as a photoactive material to provide a stable photocurrent. Constructing an S-scheme heterojunction with AgBr and BiOBr facilitates the effective separation of photogenerated carriers. Meanwhile, the introduction of La and oxygen vacancies extends the range of visible-light absorption and improves the light utilization. To strengthen the PEC performance, a cascade catalytic amplification strategy was introduced using iron-phosphate-based (FePOs) nanozymes. These nanozymes exhibit dual enzyme-mimicking activities, including catalase (CAT)-like and superoxide dismutase (SOD)-like functions, enabling the sequential disproportionation of •O₂^- into H₂O₂ and O₂, followed by the decomposition of H₂O₂ into O₂ and H₂O. The generated oxygen acts as an efficient electron acceptor, promoting the removal of photogenerated electrons and consequently boosting the PEC response. Under optimized conditions, the developed immunosensor enables highly sensitive quantification of CA15-3 (0.0005-200 U/mL) and CA125 (0.001-200 U/mL), with corresponding limits of detection (LOD) of 0.00016 and 0.0003 U/mL, respectively. This study provides a promising approach to constructing efficient S-scheme photoactive heterostructures and offers new insights into nanozyme-based cascade amplification for high-performance PEC biosensing.

In this study, a split-type electrochemiluminescence (ECL) sensor based on polypeptide cleavage was proposed for the sensitive detection of matrix metalloproteinase 2 (MMP 2). The bimetallic nanoclusters were protected by mercaptosuccinic acid (MSA), named Au₃Ag₅(MSA)₃, serving as a signal probe. Owing to the synergistic effect of the bimetal composition, the clusters exhibited enhanced ECL properties. Polypeptide chains (PLGVR) that can be specifically cleaved by MMP 2 were selected from the MMP 2 domain. Additionally, the antifouling segment (PPEKEK) and the binding segment (CCC) were incorporated into the polypeptide chain design. In the presence of MMP 2, a specific cleavage site on the polypeptide was targeted, resulting in the detachment of Au₃Ag₅(MSA)₃ and subsequent generation of an ECL signal. Compared to conventional detection methods, this approach exhibited enhanced sensitivity and improved stability. This method provides a valuable reference for detecting members of the matrix metalloproteinase family and holds promising prospects for future development.

Considering the slow kinetics of oxygen evolution reaction (OER) and the need for high potential, organic electro oxidation, which is more prone to occur at low potential, is adopted to replace OER process. The research method combined with hydrogen evolution reaction (HER) has gradually become the mainstream direction for the synergistic production of hydrogen and high value‐added organic products. In this work, the NiFeB hydroxide (NiFeB(OH)) nanosheet was prepared. Benefited from the incorporation of electron‐deficient boron (B), the NiFeB(OH) catalyst exhibited excellent catalytic activity for the electrooxidation of benzylamine (BA), with benzonitrile (BN) being successfully fabricated. The experiment further proves that the conversion from BA to BN not only has high selectivity (100%) and Faraday efficiency (94.15%), but also excellent stability, which can achieve long‐term operation. The excellent catalyst studied in this work provides new ideas and methods for the efficient production of benzonitrile, an organic intermediate.

In this Letter, a sensitive DNA sensing platform was developed using an indium-ion-coordinated 1,1,2,2-tetra(4-carboxylphenyl)ethylene (TPE) metal–organic gel (In-MOG) as an aggregation-induced electrochemiluminescence (AIECL) emitter and nanosurface energy transfer (NSET) as an efficient quenching strategy for detecting aflatoxin B1 (AFB1), the most dangerous food toxin. The coordination occurred in indium ions, and carboxyl groups restricted the internal rotation and vibration of TPE molecules, forcing them to release photons via radiative transitions. The quenchers of microfluidic-produced gold nanoparticles were embedded in a long-tailed triangular DNA structure, where the quenching phenomenon aligned with the theory of ECL-NSET under the overlap of spectra and appropriate donor–acceptor spacing. The proposed analytical method showed a sensitive ECL response to AFB1 in the wide concentration range of 0.50–200.00 ng/mL with a limit of detection of 0.17 ng/mL. Experimental results confirmed that constraining luminescent molecules using coordination and bonding to trigger the AIECL phenomenon was a promising method to prepare signal labels for the trace detection of food toxins.

The accurate discernment and separation of chiral isomers with high precision remain a significant challenge in various industries and biological fields. In this investigation, an electrochemiluminescent (ECL) chiral recognition platform was devised to ascertain the presence of phenylalanine (Phe). Notably, a homochiral [Ni₂(l-asp)₂(bipy)] (Ni-LAB) was established as a dual-function coreactant accelerator and chiral recognition substrate. Ni-LAB facilitates the reaction between the coreactant (K₂S₂O₈) and the luminescent entity 3,4,9,10-perylenetetracar-boxylic-l-cysteine (PTCA-cys), thereby enhancing the ECL luminescence efficiency and improving the sensitivity of the chiral sensor. The chiral recognition potential of Ni-LAB was assessed to differentiate between Phe chiral isomers, and the underlying mechanism was comprehensively elucidated. This system exhibited remarkable proficiency in detecting Phe enantiomers and precisely differentiating a single Phe enantiomer within a mixture, showcasing exceptional levels of selectivity, stability, and reproducibility. This study paves the way for the development of advanced chiral recognition systems, potentially revolutionizing the field of chiral sensing and discrimination.