Xianlong Zhou

Synergistic molecular potassiation and interfacial engineering enhance the cycling stability of lithium batteries under extreme low-temperature conditions.

Noble-metal-based cocatalysts remain the benchmark for interfacial charge extraction and lowering surface reaction kinetics barriers for photocatalytic water splitting, but their scarcity and cost limit scalable deployment. To search for low-cost alternatives, two-dimensional MoB nanosheets (MB) were introduced as an active, noble-metal-free cocatalyst platform. The near-ideal hydrogen adsorption free energies (|ΔGH*| ~ 0.15–0.18 eV) at Mo- and O-terminated edge sites, as well as at activated B basal-plane sites, will favor H2 evolution reaction kinetics. A Schottky-like junction forms when ultrathin MB is integrated with a semiconductor light absorber, which boosts ultrafast charge separation and transfer, as resolved by femtosecond transient absorption spectroscopy and Kelvin probe force microscopy. The universality of the MB cocatalyst in accelerating reaction kinetics was confirmed across diverse semiconductor photocatalysts. An optimized Zn3In2S6/MB hybrid (ZMB-4) achieved a remarkable H2 evolution rate of 147.1 mmol g–1 h–1 under 420 nm light, while simultaneously promoting the oxidative valorization of benzyl alcohol (121.3 mmol g–1 h–1). Evidenced by ultrafast electron sink dynamics with multi-site surface activation, this work identifies two-dimensional MoB as a low-cost and universal cocatalyst platform for producing solar fuel and value-added chemicals.

Microdroplets enable selective, catalyst-free hydrogenation of biomass molecules via self-assembly and hydrogen bonding, paving the way for sustainable, tunable transformations.

We employed dimethyl sulfoxide to modulate the interfacial water structure of Cu catalysts, thereby promoting C–C coupling to C₂H₄ in CO₂ electroreduction.

H₂-free electrochemical hydrogenation of unsaturated organic compounds has garnered considerable attention as a low-carbon and efficient alternative to conventional thermocatalytic hydrogenation. However, in a traditional electrolytic cell, the compounds need to dissolve in the electrolyte before participating in the catalytic reactions, resulting in difficulties in enhancing the compounds' yield, as well as product separation and purification. A Pd membrane reactor offers a solution to these challenges by enabling the separation of a hydrogenation reaction into electrochemical and chemical processes. Here we summarize the processes of the Pd membrane reactor which drive the electrochemical hydrogenation of unsaturated compounds including gaseous reagents. We discuss various modification strategies for Pd catalysts, including the fabrication of Pd nanodendrites, incorporation of foreign metal layers, and formation of Pd alloys with other metals. These strategies aim to enhance catalytic activity by increasing the active area and fine-tuning reactant adsorption. We place significant emphasis on using this membrane reactor to hydrogenate unsaturated bonds, including CC, CC, CN, CO, and OO bonds and highlight distinct catalysts to enhance catalytic selectivity. Finally, we provide some perspectives on the challenges and outlook for other electrochemical hydrogenation reactions through the Pd membrane reactor.

The electrochemical reduction of O₂ via a two‐electron reaction pathway to H₂O₂ provides a possibility for replacing the current anthraquinone process, enabling sustainable and decentralized H₂O₂ production. Here, a nitrogen‐rich few‐layered graphene (N‐FLG) with a tunable nitrogen configuration is developed for electrochemical H₂O₂ generation. A positive correlation between the content of pyrrolic‐N and the H₂O₂ selectivity is experimentally observed. The critical role of pyrrolic‐N is elucidated by the variable intermediate adsorption profiles as well as the dependent negative shifts of the pyrrolic‐N peak on X‐ray adsorption near edge structure spectra. By virtue of the optimized N doping configuration and the unique porous structure, the as‐fabricated N‐FLG electrocatalyst exhibits high selectivity toward electrochemical H₂O₂ synthesis as well as superior long‐term stability. To achieve high‐value products on both the anode and cathode with optimized energy efficiency, a practical device coupling electrochemical H₂O₂ generation and furfural oxidation is assembled, simultaneously enabling a high yield rate of H₂O₂ at the cathode (9.66 mol h⁻¹ g_cat⁻¹) and 2‐furoic acid at the anode (2.076 mol m⁻² h⁻¹) under a small cell voltage of 1.8 V.

Electrochemical reduction of CO2 to high-energy-density oxygenates and hydrocarbons beyond CO is important for long-term and large-scale renewable energy storage. However, the key step of the C–C bond formation needed for the generation of C2 products induces an additional barrier on the reaction. This inevitably creates larger overpotentials and greater variety of products as compared to the conversion of CO2 to C1 products. Therefore, an in-depth understanding of the catalytic mechanism is required for advancing the design of efficient electrocatalysts to control the reaction pathway to the desired products. Herein, we present a critical appraisal of reduction of CO2 to C2 products focusing on the connection between the fundamentals of reaction and efficient electrocatalysts. An in-depth discussion of the mechanistic aspects of various C2 reaction pathways on copper-based catalysts is presented together with consideration of practical factors under electrocatalytic operating conditions. By providing some typical examples illustrating the benefit of merging theoretical calculations, surface characterization, and electrochemical measurements, we try to address the key issues of the ongoing debate toward better understanding electrochemical reduction of CO2 at the atomic level and envisioning the roadmap for C2 products generation.

Hierarchical porous structures are highly desired for various applications. However, it is still challenging to obtain such materials with tunable architectures. Here, this paper reports hierarchical nanomaterials with oriented 2D pores by taking advantages of thermally instable bonds in vanadium‐based metal–organic frameworks (MOFs). High‐temperature calcination of these MOFs accompanied by the loss of coordinated water molecules and other components enables the formation of orderly slit‐like 2D pores in vanadium oxide/porous carbon nanorods (VO_x/PCs). This unique combination leads to an increase of the reactive surface area. In addition, optimized VO_x/PCs demonstrate high‐rate capability and ultralong cycling life for sodium storage. The assembled full cells also show high capacity and cycling stability. This report provides an effective strategy for producing MOFs‐derived composites with hierarchical porous architectures for energy storage.