Ran Long

Photothermal catalytic dry reforming of methane (DRM) mediated by lattice oxygen (O _l ) is promising for converting two major greenhouse gases into syngas. However, conventional oxide supports possess strong metal–oxygen bonds that restrict O _l migration, compromising stability, typically less than 200 h. Herein, we design a Rh/Mg ₂ V _1.33 O ₄ catalyst with Rh ^{δ +} ─O _v ─V ^{n +} interfacial sites ( n = 3 or 4). The defective spinel vanadate support exhibits quasi‐metallic properties, enabling efficient solar harvesting and photothermal conversion. Under 4 W cm ⁻² light irradiation without external heating, the redox flexibility of V species enables an interfacial redox shuttle (Rh ^{δ +} ─O _v ─V ^{n +} ⇌ Rh ^{δ +} ─O _l ─V ^{( n +1)+} ), which endows the catalyst with effective O _l migration and regeneration ability in the DRM reaction. This property steers the reaction along a coking‐resistant CH ₃ O* pathway and guarantees structural stability. As a result, the catalyst delivers long‐term stability for 1000 h, outperforming state‐of‐the‐art photothermal catalysts. It also achieves high syngas generation rates of 16.1 and 18.6 mol g _Rh ⁻¹ h ⁻¹ for H ₂ and CO, respectively, along with a light‐to‐chemical energy efficiency of ∼20.9%. This work establishes quasi‐metallic, redox‐active vanadate supports as a transformative platform for durable O _l ‐mediated photothermal catalysis.

Correction for ‘Unlocking the catalytic potential of heterogeneous nonprecious metals for selective hydrogenation reactions’ by Wanbing Gong et al. , Chem. Soc. Rev. , 2025, 54 , 960–982, https://doi.org/10.1039/d4cs01005a.

Polyethylene terephthalate (PET) plastic waste is highly resistant to natural degradation, and conventional chemical recycling routes typically rely on acidic, basic or hydrogen-assisted processes under harsh conditions. Here, we present a solvent-free, oxidative depolymerization strategy that converts PET plastic waste into a valuable monomer using an atomically dispersed Fe catalyst within a zeolite framework. Consequently, high-purity terephthalic acid (TPA) can be obtained with a yield of 90.7% at 260 °C under atmospheric oxygen. This conversion can also be driven using the air or solar heat. We reveal that this high efficiency is due to the reversible Fe(II)/Fe(III) redox cycle sites modulating the local oxygen environment and activating molecular oxygen to generate reactive oxygen species (ROSs). These ROSs efficiently cleave the PET ester bonds, and the reaction is sustained by hydrogen atoms derived from the polymer backbone. Meanwhile, the synergistic acid sites of the ZSM-5 framework promote substrate protonation and lower the activation energy barrier for C–O scission. This strategy could reduce net carbon emissions by 73.1% compared to conventional TPA production.

Plasmonic catalysis offers a promising route to solar-driven chemical transformations, yet its efficiency is severely limited by the high energy barrier for hot electron utilization, particularly for activating inert bonds. While recent progress suggests that the plasmonic local electric field can synergize with hot carriers to enhance reactivity, the specific contribution of the local electric field to bond activation remains unclear. Herein, we observed the visible-light-driven cleavage of the C–F bond under the intense local electric field of the Ag interparticle gaps via in situ surface-enhanced Raman spectroscopy (SERS). The relationship between nanoparticle size-dependent local electric field enhancement/hot carrier generation efficiency and C–F bond cleavage kinetics demonstrates that the local electric field can effectively lower the energy barrier for hot electron injection into adsorbate’s lowest unoccupied molecular orbital (LUMO). Density functional theory (DFT) calculations further suggest that the contribution of the local electric field (CF) to the barrier reduction is at least 25% under our experimental conditions by lowering the adsorbate LUMO level. These insights deepen the mechanistic understanding of plasmonic catalysis, such as the superlinear dependence of the reaction rate on light intensity, presenting the local electric field as a critical design parameter for high-efficiency plasmonic catalysts targeting inert chemical bond activation.

Micropollutants in aquatic environments pose a significant threat to human health, which requires new designs of photoreactor and photocatalyst for better degrading micro pollutants. Here, we have designed a flow surface concave photoreactor through 3D printing, which can improve light collection ability by reflecting light multiple times on the surface. It is combined with a single atom modified Cr‐Bi ₃ O ₄ Br/PVDF photocatalytic membrane for photo driven removal of antibiotics at environmentally relevant concentrations (100 ng L ⁻¹ to 10 mg L ⁻¹ ). The use of photocatalytic membrane flow system can effectively promote the contact between micro pollutants and active hydroxyl radicals ·OH generated in nanopores, thereby significantly improving degradation efficiency. Notably, in a 100 ng L ⁻¹ tetracycline (TC) solution, the removal rate can reach 99.9%, demonstrating the importance of designing flow‐through concave photoreactor and photocatalytic membrane. Under natural sunlight conditions, the removal rate of TC reached an impressive 99% and total 5000 mL after 5 cycles with flow velocity 1.68 mL/min. This work not only provides an effective strategy for the removal of micro pollutants driven by sunlight, but also provides important references for the design of water treatment equipment through the synergistic effect of 3D printed concave photoreactors and composite materials.

Geoelectrochemical reduction of CO₂ is proposed as a potentially significant abiotic synthesis pathway catalyzed by sulfide minerals under planetary conditions, but whether this reaction could be catalyzed by geologically abundant carbonate and phyllosilicate minerals is unknown. Here we show that adsorption of trace transition metal cations, such as Cu(II) and Zn(II), endows common Ca/Mg-carbonates and phyllosilicates with high catalytic performance for CO₂ reduction to form methane, formic acid, carbon monoxide, and C₂ organics. We also observe viable synthesis of C-N bonded compounds (mainly acetamide) when ammonia is present. During these reactions, the adsorbed metal cations are partially reduced into metallic states and become catalytic, while mineral substrates facilitate the water dissociation to supply protons for CO₂ hydrogenation. This facile electrochemical reduction of CO₂ catalyzed by carbonates and phyllosilicates could facilitate the origin of life on the primitive Earth and help explain the detection of organics on other habitable planetary bodies.

Electrified chemosynthesis shows great promise for sustainable chemical manufacturing. However, the reaction efficiency in continuous flow electrochemistry is currently unsatisfactory due to restricted mass transport at the two-phase boundary. Here we present an effective flow management strategy involving electrolyzer structural optimization to intensify the localized electrochemical process. We demonstrate this approach using the electrosynthesis of cyclohexanone oxime from cyclohexanone and nitrite as a representative example. The cathodic counterpart is regulated by a flow-through channel architecture that drives the significant electrolyte convection throughout the porous electrode matrix and minimizes the hydrodynamic diffusion distance, giving the catalyst full accessibility to the feedstock. Using an optimal cobalt single-atom catalyst, we demonstrate the oxime electrosynthesis with a Faradaic efficiency of over 95%, regardless of the operating conditions. Furthermore, we achieve a high single-pass conversion efficiency of up to 95% by balancing the supply of feedstocks between cyclohexanone and in situ generated hydroxylamine through subtle control of the electrolyte flow rate. This continuous-flow electrosynthesis process demonstrates long-term stability, operating for up to 110 hours without the loss of activity, which highlights its great potential for practical implementation.

We demonstrate that N-sites on N-doped graphene/TiO ₂ act as nitrogen carriers, sustaining NH ₃ generation via a N-cycle. Nitrogen is detached from graphene for NH ₃ synthesis and replenished by atmospheric N ₂ .

Lattice oxygen (O_l)-mediated photothermal dry reforming of methane (DRM) offers a promising approach to converting two greenhouse gases (CH₄ and CO₂) into syngas. However, the intrinsic stability of metal-oxygen bonds often restricts the O_l mobility. Herein, we developed a Ru/BaTiO₃ with a well-defined metal-support interface that enables a photoinduced lattice oxygen spillover effect for efficient and stable photothermal DRM. Under light irradiation, the photoexcited electrons transfer to Ru^δ+ sites, greatly improving its electron density, while the photogenerated holes move to the lattice oxygen of BaTiO₃, which weakens the Ba-O-Ti bonds for facilitating lattice oxygen migration. In situ characterizations and theoretical calculations confirm that this photoinduced lattice oxygen spillover effect promotes reactant activation and shifts the DRM pathway from the carbon-forming CH₃* route as observed in thermal catalysis to a carbon-free CH₃O* route, thereby effectively suppressing coke formation. As a result, the Ru/BaTiO₃ catalyst exhibits excellent catalytic stability (>120 h) and superior catalytic activity (10.1/11.4 mol g_Ru^-1 h^-1 for H₂/CO production) under simulated sunlight irradiation. This work motivates the design of efficient and stable DRM catalysts under mild conditions.

Electrocatalytic oxygen reduction reaction (ORR) near its thermodynamic equilibrium potential is vital for efficient energy conversion. However, low-valent metal ions generated at high cathodic potentials are typically required to achieve effective O₂ activation. Herein we report O₂ activation promoted by a Sc³⁺-hung Co^III corrole, which realizes markedly boosted ORR electrocatalysis. Co^III corrole 1 with an appended crown ether substituent was synthesized. By grabbing a Sc³⁺ ion, the ORR overpotential with Sc³⁺-hung 1 decreased by 1.0 V in acetonitrile and 170 mV in 0.5 M H₂SO₄ solutions. Importantly, Sc³⁺-hung 1 achieved an ORR half-wave potential of 0.78 V vs RHE in 0.5 M H₂SO₄ solutions with a transferred electron number of 3.87. Our results suggest that the hanging Sc³⁺ promotes O₂ binding and activation at the Co^III ion of 1 to generate a Co^III-superoxo-Sc³⁺ corrole cation radical and assists subsequent O-O bond cleavage by accepting the leaving hydroxide.