Juncai Dong

The oxygen evolution reaction (OER) is pivotal for diverse electrochemical energy conversion systems; however, it has so far been plagued by sluggish kinetics and excessive energy consumption. In this study, we proposed an innovative thermoelectric‐electrocatalytic coupling strategy to enhance OER efficiency by constructing an Ohmic heterointerface through uniform integration of RuO ₂ with thermoelectric oxide (PrCoO ₃ ). Combined experimental and theoretical analyses revealed that the thermoelectric potential generated by PrCoO ₃ selectively activates the intrinsically inert (101) facet of RuO ₂ by lowering *OOH formation barrier, thereby substantially boosting the overall OER performance. Consequently, the RuO ₂ /PrCoO ₃ heterointerface delivered exceptional OER performance under a mild temperature gradient (Δ T ) of 175°C, achieving dramatic reduction in overpotential at 10 mA cm ⁻² from 300 mV (Δ T = 0°C) to 178 mV, 4 300% increase in current density, and negligible potential loss over 1,000 h. When the catalyst was assembled into an anion exchange membrane water electrolyzer, the cell driven by spontaneous heating reached a low voltage of 2.18 V at a current density of 2.0 A cm ⁻² , with stable operation for 600 h. These insights into harnessing thermal gradient via integrated electrocatalytic system are crucial for the recovery of industrial waste heat and its conversion into high‐value chemicals.

Synergistic spin-state and local coordination engineering offers a promising strategy for enhancing the acidic oxygen reduction reaction performance of Fe–N–C electrocatalysts, yet the precise control and stabilization of active sites remain challenging. Here we report a Fe–La geminal-atom electrocatalyst (Fe₁-La₁/NC) with spontaneous ferromagnetic spin ordering for acidic oxygen reduction reaction. The catalyst achieves a half-wave potential of 0.92 V and a turnover frequency of 17.3e^-site⁻¹s⁻¹, compared with commercial Pt/C (0.87 V, 9.9e^-site⁻¹s⁻¹). A proton exchange membrane fuel cell equipped with Fe₁-La₁/NC cathode delivers a high current density of 56 mA cm⁻² at 0.9V_iR-free under H₂-O₂ condition, while maintaining stable operation for 100 h at 0.67 V with 86% performance retention. Operando studies and theoretical simulations reveal that La incorporation promotes a spin-polarized high-spin Fe 3 d configuration and room-temperature ferromagnetic ordering, while also regulating the local coordination/electronic structure and oxygen-intermediate adsorption. Moreover, La enables dynamic self-adaptive stabilization of Fe sites, which mitigates the conventional activity–stability trade-off. This finding provides an avenue to rationally design efficient and selective electrocatalysts.

Direct 3d–4f orbital coupling engineered by confining Cu–Er pairs in paddlewheel frameworks strengthens *CO adsorption and lowers the *CO → *CHO barrier, enabling efficient CO ₂ electromethanation with 82% CH ₄ faradaic efficiency.

Achieving stable and efficient alkaline water electrolysis (AWE) under fluctuating renewable energy inputs is essential for large-scale green hydrogen production. However, frequent shutdown-induced reverse current (RC) effects pose significant challenges to electrode durability. Here, we introduce a gradient interlayer engineering strategy to develop robust AWE electrodes that intrinsically resist both electrochemical reconstruction and mechanical fatigue. By constructing a dense interlayer with Ni(112̅)/Ni₃S₂(1̅20) heterointerfaces, the electrode demonstrates high catalytic activity (1.79 V @1000 mA cm^-2─meeting the U.S. DOE 2026 target), excellent operational stability (>1500 h at 1000 mA cm^-2 in 30 wt % KOH at 80 °C), and exceptional RC resistance for 3600 accelerated startup/shutdown cycles. Mechanistic studies through cross-sectional characterizations and theoretical calculations reveal that the seamless interlayer at the catalyst-substrate interface enhances interfacial adhesion, mitigates lattice mismatch, and facilitates charge redistribution, ensuring robust stability and integrity even under operational strains and potential reversals. This work establishes interface crystallography as a design paradigm for durable electrodes, potentially overcoming the stability-activity dilemma toward industrially relevant electrolyzers coupled with fluctuating renewable energy sources.

By varying the mass ratio of the amphiphilic triblock copolymer (P123) to 1,3,5-trimethylbenzene (TMB), alongside the content and molecular weight of polyethylenimine (PEI) and the incorporation of catalyst ammonium fluoride (NH4F), four distinct types of polyethylenimine-modified siliceous mesostructured cellular foam (PEIs-MCF) are prepared. To elucidate the annihilation mechanism of positrons and positronium within the amorphous porous materials, we perform positron age-momentum correlation techniques (AMOC). The Doppler broadening spectroscopy results obtained from AMOC indicated differences in electronic momentum across porous materials with varying free volume holes following PEI impregnation. Based on the differentiation of the S parameters for samples with different free volume hole sizes, −NH2 concentrations and the structural forms of −NH2 in the branches of PEI, various annihilation processes of positrons within the age domain were explored. Employing positron annihilation lifetime spectroscopy (PALS), the study examined the relationship between PEI content and the pick-off annihilation rate of o-Ps as PEI was introduced. According to the examination of correlation of the positron annihilation linear parameter S derived from DBS data extracted from AMOC and the o-Ps intensity from PALS measurements (S-Io‑Ps) and the discussion in the authors’ previous work, the chemical environments of PEIs-MCF modified with low content of PEI differ from those of PEIs-MCF modified with high PEI content.

The cluster-plus-glue-atom model was innovatively employed to design Ru–Sn oxide catalysts, investigating the role of Sn as glue atoms in modifying OER performance.

High‐entropy transition metal oxides with a spinel structure exhibit excellent catalytic activity for the redox reactions of sulfur species in lithium‐sulfur batteries (LSBs). However, the underlying origin of their catalytic activity—driven by geometric configuration and electronic structural evolution—remains unclear. Herein, it is applied X‐ray absorption fine structure (XAFS) spectroscopy, complemented by ex situ X‐ray photoelectron spectroscopy analysis and theoretical calculations, to establish the structure‐activity correlation of the catalyst. Using spinel‐structured Co ₃ O ₄ as a model catalyst, two systems are constructed as LSB catalysts, specifically a medium‐entropy oxide, (FeCoNi) ₃ O ₄ , and a high‐entropy oxide (HEO), (FeCoNiMnZn) ₃ O ₄ , by incorporating different metal elements to modulate the ratio between Co‐occupied octahedral (Co _Oct ) and tetrahedral (Co _Tet ) sites. XAFS experiments and theoretical analyses reveal the geometric configuration and electronic structural evolution of HEO catalysts. Meanwhile, the octahedral site is recognized as the primary active center. Additionally, the weakened covalency (strengthened polarity) of the Co _Oct –O bonds in the HEOs serves as the origin of the enhanced redox kinetics of reversible polysulfide conversion, which is supported by theoretical calculations. This work provides new insights into the catalytic mechanism of the spinel‐structured high‐entropy transition metal oxide electrocatalysts, thereby facilitating the rational design of highly efficient electrocatalysts for advanced LSBs.

Breaking the known activity-stability trade-off is essential for the broad implementation of Fe-N-C catalysts in fuel cells. Here, we report the development of an atomically dispersed Fe-N-C catalyst with highly active FeN_x sites on carbon support with dispersed graphitic microdomains (FeN_x-Gmd), which were generated during the Fe₃C-catalyzed graphitization. The introduction of graphitic microdomain makes the FeN_x-Gmd exhibit outstanding oxygen reduction reaction activity when used as a cathode catalyst in practical fuel cells, with impressive peak power densities of 1.06 and 0.55 W cm^-2 under 150 kPa_abs H₂/O₂ and H₂/air, respectively. Both power densities proved that the FeN_x-Gmd were among the top five best-reported non-PGM-based catalysts. Theoretical calculations suggested the FeN_x sites supported on carbon structure with fewer defects, corresponding to a higher graphitic degree, showing higher activity compared to the one with more defects. Moreover, the improvement in catalyst activity does not compromise stability since graphitic microdomains enhanced the corrosion resistance of the carbon support. As a result, after 10000 cycles of accelerated stability test, the FeN_x-Gmd can still deliver a peak power density of 0.79 W cm^-2 in the H₂/O₂ test, which was even higher than many catalysts at the initial stage. Unlike the reported strategy of reducing the ratio of more active but less stable pyrrolic N-coordinated Fe (S1) sites, this study provided an alternative pathway for breaking the activity-stability trade-off of the Fe-N-C catalyst without significantly reducing the ratio of S1 sites.