Latest ArticlesThe zinc-air battery (ZAB)-hydrogen peroxide (H2O2) generation system produces H2O2 through a 2-electron oxygen reduction reaction (ORR) at the ZAB air cathode while simultaneously providing external electrical power. This system offers a promising, eco-friendly solution for both energy storage and chemical production. Despite its promise, a comprehensive review of this topic is still scarce. To fill this void, this review discusses the background and mechanisms of the ZAB-H2O2 generation system and covers approaches to achieving efficient and stable operation through 2e− ORR catalyst design and optimization, the regulation of the electrolyte, cathode configuration design, and electrochemical operating conditions. From the perspective of the cathode, anode, electrolyte, and their integration with energy systems, this review systematically analyzes the key challenges and optimization strategies. In addition, this review summarizes the main technical bottlenecks this system faces and proposes potential solutions and development suggestions for future research and practical applications.
Glycerol oxidation reaction has got lots of attention in an electrocatalytic system of simultaneous hydrogen production and valuable chemicals generation. However, the lack of electrochemical dehydrogenation capability of the active phase is hard to deliver a large current density at a low potential. Furthermore, high selectivity of products is also still far from being completed due to the adsorption-desorption disequilibrium of glycerol and the obtained products, reducing the economic feasibility and limiting the practical application. Here, we propose a strategy to boost the electrocatalytic glycerol oxidation through electron-deficient Ni sites induced by electron transfer of heterojunction interface. Taking Ni3S2/Cu2S as a pre-catalysts, we demonstrate that the electron-deficient Ni site can favor the dehydrogenation of the active phase to facilitate the rapid transformation of Ni2+/Ni3+ in the electrooxidation process of glycerol. Furthermore, electron deficient Ni sites balance competitive adsorption of active species, improving the activity and selectivity of glycerol oxidation. As expected, the electrocatalysts exhibit selectivity of 93.3% for formate at the 1.35 V, and require only 1.45 V to drive an industrial-level current densities of 600 mA/cm2. This work provides valuable insights into constructing highly active and selective electrocatalysts for organic electrosynthesis in hybrid water electrolysis.
Developing non-precious electrocatalysts with high-efficiency hydrogen evolution reaction (HER) activity for hydrogen production at all pH values is crucial for the application and promotion of water electrolysis. Herein, a unique structure of nickel-cobalt (Ni–Co) nanoparticles@Ni0.19Co0.26P nanowires core/shell arrays on Ni foam as a pH-universal electrocatalyst for hydrogen evolution is synthesized by a simple hydrothermal process and thermal reduction treatment. The morphological analysis reveals that numerous Ni–Co nanoparticles are densely packed inside the hollow interior of Ni0.19Co0.26P nanowires. This unique structure integrates the advantages of high surface area from the nanowires and enhanced electronic conductivity from the Ni–Co nanoparticles, effectively addressing the conventional issue of slow charge transfer rate in 3D metal-based compounds, which is typically caused by a long transfer distance. The electrocatalysts provide an excellent hydrogen evolution reaction performance in alkaline, neutral, and acidic media with an overpotential of 35, 36, and 23 mV to reach the current density of 10 mA/cm2, respectively. This study highlights the potential of Ni–Co nanoparticles@Ni0.19Co0.26P nanowires as a cost-effective and pH-universal HER electrocatalyst, offering promising prospects for sustainable hydrogen production.
Scarce investigations have focused on coinage metal clusters possessing fixed cores but varying binding ligands in the context of catalysis. Here in this work, we successfully employed two types of carboxylic acid-based molecular tweezers to selectively capture two Cu6 clusters (Cu6-a and Cu6-b). Cu6-a and Cu6-b have identical cluster cores but different protected ligands, therefore provide accurate platform for investigating ligand effects in cluster catalysis. Notably, Cu6-b represents a rare example of a two-directional rod framework, marking the first instance of such a structure in coinage metal cluster-based MOFs. The integration of oxygen within OBB significantly enhances local spatial polarization, facilitating the charge separation and ROS generation efficiency of Cu6-b under visible-light irradiation. Consequently, the oxygen-containing Cu6-b exhibits superior photocatalytic performance in the aerobic oxidation of sulfide, achieving both high yield and selectivity. This work provides a valuable approach for precisely control the Cu clusters structures to regulate their properties.
Ultraviolet (UV) nonlinear optical (NLO) crystals have received substantial interest in advanced laser technology. However, tailoring a UV NLO material with a large second harmonic generation (SHG) response and good UV transparency remains a challenge. Here, inspired by the classic A3-RE2-[BO3]3 parent template, two new rare-earth borate NLO crystals, RbNa2La2(BO3)3 (RNLBO-Ⅰ) and Rb0.681Na2.319La2(BO3)3 (RNLBO-Ⅱ), were extracted by merging larger ionic radius cations Rb+ and La3+ simultaneously using a chemical substitution-oriented strategy. As expected, both compounds achieve significant enhancements in SHG activities, reaching 4.5 × and 4.3 × KDP, respectively, exceeding three times that of the isomorphic Na3Gd2B3O9. Notably, RNLBO-Ⅰ displayed the highest SHG response among alkali metal RE-borate NLO crystals containing isolated [BO3] groups in the short-wave UV region. Moreover, RNLBO-Ⅰ and -Ⅱ demonstrated short UV cutoff edges at 213 and 207 nm, corresponding to wide bandgaps of 5.3 and 5.6 eV, respectively. Additionally, theoretical calculations and dipole moment analysis were conducted to clarify the origin of the enhanced SHG activities of RNLBO-Ⅰ and -Ⅱ. The optimal balance between SHG intensity and UV transparency in RNLBO-Ⅰ and -Ⅱ underscores their potential as UV NLO candidates and offers valuable insights for fabricating new advanced UV NLO materials.
Polyoxometalate-based metal-organic complexes (POMOCs) which combine the structural features and performance advantages of MOCs and POMs, have a wide application in the field of catalysis. However, the catalytic capacity of POMOCs commonly cannot be fully utilized due to their imporosity and low surface area of single-crystals. In this work, a new POMOC with a formula of [Cu3O(4-atrz)6(PO3)(PMo12O40)] (POMOC 1, 4-atrz = 4-amino-4H-1,2,4-triazole) was synthesized. And the size regulation of POMOC 1 from single-crystal to nanoscale was achieved by using citric acid as a modulator and adjusting the reaction temperature. Nano-sized POMOC 1 exhibited excellent catalytic performance in the oxidation reaction of phenols owing to the synergistic catalysis of POM and coordinatively unsaturated Cu(Ⅱ), and more surface-accessible catalytic sites of nano-catalyst.
Oxygen (O) doping is a promising strategy for enhancing the air stability and lithium metal compatibility of sulfide solid electrolytes (SSEs). However, the impact of various O sources on the structure and properties of SSEs remains unclear. In this study, we synthesized a series of O-doped electrolytes, Li5.5PS4.5-xOxCl1.5 (LPSCOx, 0.1 ≤ x ≤ 0.5), using Li2O and P2O5 as O sources, and systematically investigated their differences in structure, air stability, and electrochemical properties. O preferentially substitutes sulfur (S) at the 16e site and begins to replace S at the 4d site once a certain O concentration is reached. Notably, the P2O5-doped electrolytes (P-LPSCOx) exhibit a greater oxygen tolerance content (0.24) at the 16e site, along with better air stability, higher ionic conductivity, and superior lithium metal compatibility. XRD, SEM, and XPS analyses reveal that the P2O5-doped electrolytes exhibit larger cell parameters, higher densification, and fewer side reactions with lithium metal compared to the Li2O-doped counterparts. This study provides valuable insights into the development of high-performance O-doped sulfide electrolytes.
Oxygen evolution reaction (OER) is a key reaction in proton exchange membrane water electrolyzers (PEMWEs). Therefore, developing cost-effective acid-stable electrocatalysts to drive efficient OER is crucial. Here, we constructed a RuO2 electrocatalyst (MoB-RuO2) co-doped Mo and B atoms, which exhibits excellent OER performance in acidic media. In 0.5 mol/L H2SO4, MoB-RuO2 exhibited a very low overpotential (166 mV) and could be operated stably for more than 550 h at 10 mA/cm2 current density without significant loss of activity. More than 240 h of stable operation at 200 mA/cm2 current density was achieved when using MoB-RuO2 as a PEMWE anode. Experimental and theoretical results demonstrated that the excellent OER activity and stability of MoB-RuO2 mainly originated from the incorporation of B atoms leading to the coordination unsaturation of the active centre Ru, and the simultaneous doping of Mo and B atoms modulated the electronic structure of Ru, which lowered the covalency of the Ru-O bond, thus making the catalyst exhibit excellent stability.
The immense potential of one-dimensional (1D) hybrid lead halide perovskites (HLHPs) in single crystal X-ray detection is hindered by their relatively low charge transport abilities and needle-like morphology. Alloying mixed cations in 1D HLHP is expected to realize superior charge mobility and large single crystals. Herein, we report a 1D HLHP of (ATZ)(EA)4Pb3I11 (1) with thiazol-2-aminium (ATZ)+ and ethanaminium (EA)+ as the mixed cations, demonstrating an exceptional 1D HLHP for high-performance X-ray detector. The H···I hydrogen bonds with a fraction of 69.7% are stronger than those in 1D HLHPs containing solely (ATZ)+ or (EA)+ cations. The single crystal of 1 posesses remarkable semiconducting properties, including a high resistivity (1.94 × 1011 Ω cm) and a large mobility-lifetime product (2.22 × 10−4 cm2/V), which contribute to the outstanding X-ray detection, manifested by a high sensitivity of 1356 µC Gyair−1 cm−2 and an ultra-low dark current drift of 5.01 × 10−8 nA cm−1 s−1 V−1.
Reactive oxygen species (ROS)-based endoplasmic reticulum (ER) stress is a prerequisite for the induction of immunogenic cell death (ICD), and the development of metal-based ICD inducers has garnered significant attention. However, the drug-target mechanisms of ICD inducers still require further exploration. Herein, we reported an ER-targeting iron(Ⅱ) complex (Fe-NBM) as an ICD inducer, which was obtained through a solvothermal domino reaction. Accordingly, pyridin-2-ylmethanamine and 1-methyl-2-formylbenzimidazole underwent consecutive covalent transformations to form a novel N-heterocyclic ligand, which subsequently coordinated with ferrous chloride to directly yield the crystalline Fe-NBM in one pot. Confocal laser scanning microscope (CLSM), molecular docking and cellular thermal shift assay (CETSA) showed that Fe-NBM could specifically target the ER by binding to the IRE1α (Inositol requiring kinase enzyme 1 alpha) and induce ICD by generating ROS-based ER stress. In an immunocompetent mouse model, Fe-NBM could significantly inhibit tumor growth and stimulate anti-tumor immunity, and exhibit an enhanced effect when combined with anti-PD1 therapy, leading to near-complete tumor elimination. To gain deeper understanding of how to synthesize such effective ICD inducers at the molecular level, a combination of electrospray ionization mass spectrometry (ESI-MS) and crystallography was employed for thoroughly tracking the step-economy synthetic process. To the best of our knowledge, Fe-NBM is the first iron-based ICD inducer that directly targets ER through binding to IRE1α. We believe that the ICD-related target information presented in this work will enhance our understanding of the molecular mechanisms underlying ICD and facilitate the design of new ICD inducers.
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