Shun Lu

The growing accumulation of poly(ethylene terephthalate) (PET) waste and the increasing demand for clean hydrogen call for integrated electrochemical strategies. Ethylene glycol oxidation reaction (EGOR), derived from PET hydrolysis, offers a thermodynamically favorable alternative to the sluggish oxygen evolution reaction (OER) and can be coupled with the hydrogen evolution reaction (HER) to simultaneously produce value-added chemicals and H2. This review provides a system-level overview of EGOR||HER paired electrolysis, spanning reaction fundamentals, catalyst design, cell configuration, and future challenges. First, the competing EGOR pathways toward C1 products (such as formate/formic acid) and C2 products (such as glycolate/glycolic acid) are discussed. Key energetic descriptors, including cell voltage, overpotential, Faradaic efficiency, and energy efficiency, are then summarized to clarify the advantages of replacing OER with EGOR. Recent advances in catalysts, including precious metals, transition-metal compounds, metal–organic frameworks (MOFs), organic catalysts, and hybrid systems, are reviewed with attention to their bifunctional or compatible activity for EGOR and HER. Reactor design is further discussed by comparing single-cell and dual-cell H-type reactors with membrane-free and membrane-separated flow-cell reactors, emphasizing their different roles in mass transport, product separation, and scale-up feasibility. Finally, remaining challenges and future directions are proposed, including C1/C2 selectivity, downstream separation, impurity tolerance, catalyst durability, and practical reactor optimization. This review aims to guide the development of efficient EGOR-assisted hydrogen production systems for sustainable PET electro-upcycling.

The commercialization of fuel cells is severely impeded by the sluggish kinetics of oxygen reduction reaction (ORR) and instability of conventional Pt/C catalysts, primarily due to weak metal-support interactions. Here, we propose an interfacial charge engineering strategy to construct robust Pt-Mo ₂ C heterostructures on nitrogen-doped carbon. Synthesized via a scalable, in-situ concurrent pyrolysis-reduction, the nanocomposite features precisely modulated electronic coupling. X-ray absorption fine structure spectroscopy confirms strong interfacial interaction, delineated by a distinct Pt-Mo bond (~ 2.72 Å) and a high Pt-Mo coordination number (~ 1.81). Theoretical calculations demonstrate that this heterostructured interface functions as an electronic reservoir, driving directional charge redistribution. This transfer downshifts the d -band center of interfacial Pt atoms, thereby optimizing the binding strength of oxygenated intermediates and accelerating ORR kinetics. Electrocatalytic measurements reveal that the engineered Pt-Mo ₂ C/NC catalyst delivers an outstanding mass activity of 0.65 A mg ^− 1 Pt at 0.9 V, outperforming commercial Pt/C by a factor of 4.8. Moreover, the robust Pt-Mo ₂ C coupling effectively suppresses Pt dissolution and agglomeration, endowing the catalyst with exceptional durability, retaining ~ 90% of its mass activity after 20,000 potential cycles. These results offer a general design principle for active, durable electrocatalysts based on targeted interfacial electronic modulation.

Electrolytic water splitting is a pivotal strategy for scalable hydrogen production, yet its efficiency is hindered by the sluggish kinetics of the oxygen evolution reaction (OER). Herein, we report a Ce-doped NiFe LDH-MOF nanohybrid successfully synthesized via a facile one-pot solvothermal route. This integrated architecture synergistically combines the structural robustness of layered double hydroxides (LDHs) with the expansive porosity of metal−organic frameworks (MOFs). Electrochemical assessments reveal that Ce incorporation markedly enhances OER proficiency, requiring a minimal overpotential of merely 262 mV to drive 100 mA cm-2, a 64 mV reduction relative to the undoped counterpart. Furthermore, the catalyst exhibits exceptional durability for over 100 h without perceptible degradation. Mechanistically, the unique 4f configuration and Ce3+/Ce4+ redox couple are proposed to modulate the local electronic environment and promote oxygen vacancy-related defects, thereby increasing the contribution of lattice oxygen mechanism (LOM) processes during OER. This work underscores the judicious engineering of doped nanohybrids for next-generation electrocatalysis.

Anti-swelling hydrogel and solvent-modulated MOF derivatives composite was integrated to wirelessly monitor TBHQ.

This work provides a comprehensive overview of reaction pathways, catalyst design principles, and integrated paired-electrolysis strategies for EG electro-oxidation.

Single‐crystalline Ni‐rich cathodes are regarded as promising candidates for high‐energy‐density lithium‐ion batteries (LIBs), providing superior mechanical and structural stability compared to polycrystalline counterparts. In this work, we present a low‐temperature grain‐boundary‐elimination approach to synthesize single‐crystalline LiNi _0.9 Co _0.08 Al _0.02 O ₂ (SC‐NCA) through Sn‐assisted modification. Beyond enabling low‐temperature synthesis, the integrated Sn serves a dual‐protective function. Bulk Sn doping robustly pins lattice oxygen and mitigates harmful irreversible phase transitions, preserving structural integrity. Simultaneously, the residual formation of a highly conductive Li ₂ SnO ₃ surface layer accelerates Li ⁺ diffusion kinetics and robustly passivates the cathode‐electrolyte interphase against parasitic degradation. Consequently, this dual‐site modified SC‐Sn‐NCA90 cathode exhibits exceptional electrochemical performance, delivering a remarkable capacity retention of 86.7% after 500 cycles at 1 C (2.8–4.5 V), vastly eclipsing the 40.8% retention of the polycrystalline benchmark. This work presents a low‐temperature strategy for synthesizing SC‐NCA combined with Sn doping, facilitating the development of Ni‐rich layered cathodes for high‐energy‐density LIBs.

The urea oxidation reaction (UOR), as a multi‐electron coupling reaction, provides an efficient route for treating urea‐containing wastewater and a sustainable strategy for energy‐saving H2 production. Nickel‐based catalysts attract attention due to their low cost and favorable activity, but single‐metal catalysts still suffer from limited activity and stability. To overcome these limitations, researchers enhance performance through doping, structural regulation, and composite strategies. Tungsten (W), with high electronegativity, multivalence, excellent conductivity, and environmental friendliness, is widely incorporated into nickel‐based catalysts to modulate electronic structure, improve adsorption and conversion of intermediates, and enhance stability. This review summarizes recent progress in W‐based UOR catalysts, focusing on reaction mechanisms, structural regulation strategies, and performance improvement approaches. Current challenges include active site identification, catalyst stability, reaction selectivity, and the lack of standardized evaluation protocols. Future research directions involve elucidating catalytic mechanisms, optimizing material design, establishing unified evaluation standards, and developing high‐performance W‐based composites, aiming to advance UOR applications in energy conversion, wastewater treatment, and sensing.

LiNi0.5Co0.2Mn0.3O2 (NCM523) is a mainstream lithium-ion battery cathode material with high specific capacity, which is widely applied in energy storage and power batteries. Nevertheless, it suffers from transition-metal dissolution, structural phase transition, and interfacial side reactions during long cycling, causing rapid capacity fading and inferior stability, which restricts its large-scale application. Traditionally, the Al2O3 coating layer can effectively isolate the cathode material from direct contact with the electrolyte, alleviate electrolyte decomposition, and suppress transition-metal dissolution as well as interfacial side reactions. However, the underlying charge-transfer-driven bonding mechanism between the coating layer and cathode substrate remains insufficiently understood. Herein, a sol–gel method was used to prepare Al2O3-coated NCM523 with an optimal 1.0 wt % coating content. Electrochemical tests show that 1.0 Al-NCM delivers an initial discharge capacity of 177.1 mAh g–1 at 0.2 C, retains 80.3% capacity after 200 cycles at 0.5 C (8.4% higher than bare NCM523), and exhibits 138.2 mAh g–1 at 5 C. Beyond the conventional physical protection effect of the Al2O3 coating layer, X-ray photoelectron spectroscopy, synchrotron X-ray absorption spectroscopy, and density functional theory calculations reveal a charge-transfer-driven interfacial bonding mechanism between the Al2O3 coating layer and NCM523 substrate, featuring the formation of strong Al–O–TM bonds. The charge transfer across the interface promotes Al–O–TM bonding and regulates the surface electronic structure, thereby enhancing the structural reversibility and cycling stability of the layered cathode. These findings provide new insights into the active role of the Al2O3 interfacial layer in regulating surface chemistry and enhancing the structural stability of layered oxide cathodes.

The catalytic reduction of toxic nitroaromatics to valuable amines is crucial for wastewater resource recovery, yet conventional catalysts suffer from active-site agglomeration and inadequate electronic modulation. Here, a sandwich-structured HNT@Au–CeCo nanoreactor was designed via interfacial confinement and bimetallic oxide synergy. Amino-functionalized halloysite nanotubes (HNTs) directionally anchored ultrafine Au nanoparticles, which were then coated in situ with an oxygen-vacancy-rich CeO2–Co3O4 shell. This catalyst achieved an apparent rate constant of 1.37 min–1 in reducing p-nitrophenol, representing superior improvement over the uncoated and single-oxide-coated counterparts. It also exhibited a low activation energy of 20.68 kJ mol–1 and a high turnover frequency of 825 h–1, outperforming most reported analogues. The catalyst demonstrated robust stability, broad substrate applicability in various nitroaromatics, excellent continuous-treatment capability, and effective retention of Au sites. Mechanistic studies revealed that the CeO2–Co3O4 heterojunction induced strong metal–support interaction and interfacial charge redistribution, accelerating electron transfer and the formation of active Au–H species at defect sites. DFT calculations identified the key reactive sites on the pollutant molecules during the reduction process. The ECOSAR assessment confirmed the efficient conversion of toxic nitroaromatics into low-toxicity products. This work provides an effective interfacial engineering strategy for designing high-performance nanocatalysts for environmental remediation.