Sujing Li

The morphology and microenvironment of ion-conducting polymers (ionomers) on the catalyst electrode surface critically govern the CO2 electrocatalytic performance. Herein, we report a dual-reconstruction strategy that synergistically tailors the surface structure of the Nafion ionomer using positively charged molecules and solvent effect. By combining a low-dielectric-constant solvent (isopropanol) with arginine cations, the optimized electrode achieves an 83.6% Faradaic efficiency for multicarbon (C2+) products at a high current density of –500 mA cm–2 in 1 M KOH. Based on experimental characterization and MD simulations, we propose a structural model in which the Nafion side chains are oriented away from both the catalyst surface and the electrolyte phase. In situ spectroscopic analyses, theoretical calculation, and experimental evidence suggest that this structural reorganization disrupts the interfacial hydrogen-bonding network, suppresses the competing hydrogen evolution reaction, improves effective gaseous CO2 accessibility, and facilitates C–C coupling along an energetically favorable *OC–COH pathway. This work provides valuable insights into microenvironment engineering of ionomer–catalyst interfaces for efficient CO2 electrolysis.

The development of efficient catalysts for chlorinated volatile organic compound (CVOC) abatement remains challenging due to insufficient low-temperature activity, chlorine poisoning susceptibility, and toxic byproduct formation. This study addresses these limitations through rational design of Cr-Zr codoped ceria catalysts for efficient, stable, and low-toxic degradation of chlorobenzene (CB). The optimized (CeCr)₃Zr₁ catalyst demonstrates exceptional performance, maintaining >90% CB conversion over 24 h at 240 °C with minimal polychlorinated byproducts. Structure-performance mechanistic investigations reveal that Cr-Zr doping modulates Ce-O bond strength and generates high-density oxygen vacancies, enhancing lattice oxygen mobility and reactive oxygen species generation for deep oxidation. Concurrent Zr incorporation introduces Brønsted acid sites that promote HCl formation via proton-assisted Cl removal, effectively suppressing electrophilic chlorination of aromatic intermediates. These improvements of dual oxygen-chlorine channels reduce the occurrence of electrophilic chlorination reactions in intermediate products, thereby inhibiting the formation of polychlorinated byproducts, making it more promising for industrial applications.

Industrial carbon dioxide (CO₂) phase change absorbents often face challenges in initiating phase transition and exhibit slow phase separation and sluggish reaction kinetics, particularly under variable operating conditions. To overcome these limitations, this study develops a novel ionic liquid-based nanofluid absorbent engineered for enhanced performance and operational stability. The system integrates the functionalized ionic liquid [tetraethylenepentamine][1,2,4-triazole], which offers high CO₂ loading and reliable phase transition behavior along with titanium dioxide nanoparticles and an optimized solvent mixture of 1-methoxy-2-propanol and water. The nanofluid design dramatically reduces the phase separation time by 53.85% and increases the regeneration efficiency from 79.59% to 91.72%. The key to this enhancement lies in the nanoparticles, which suppress droplet coalescence and stabilize the phase interface through surface activation, Brownian motion, and microconvection effects while decreasing mass-transfer resistance in the liquid by 38.0% and enhancing both thermal conductivity and thermal diffusivity. Moreover, the nanofluid demonstrates exceptional stability over 60 consecutive cycles, exhibiting less than 20% total performance degradation throughout the entire testing period. A successful 168 h continuous 4 Nm³·h^-1 bench-scale operation confirms its more desirable CO₂ capture capability and phase change behavior, achieving a record-low regeneration energy consumption of 1.81 GJ·t CO₂^-1. Life-cycle assessment also confirms its superior environmental sustainability versus monoethanolamine technology.

One approach for closed-loop plastics recycling relies on reverting polymers back into monomers because one can then make new plastics without loss of properties. This depolymerization requirement restricts the molecular design to making polymers with high mechanical performance. We report a three-dimensional (3D) printing chemistry through stepwise photopolymerization by forming dithioacetal bonds. The polymerized network can be transformed back into a photoreactive oligomer by dissociation of the dithioacetal bonds. This network-oligomer transformation is reversible, therefore allowing circular 3D printing using the same material. Our approach offers the flexibility of making modular adjustments in the design of the network backbone of a polymer. This allows access to fully recyclable elastomers, crystalline polymers, and rigid glassy polymers with high mechanical toughness, making them potentially suitable for diverse applications.

Solid acid catalysts (SACs) have attracted significant attention for their role in enhancing the carbon capture desorption process, primarily due to their active acid sites. By employing a synergistic strategy involving acid anchoring and structural design, both the catalytic activity and durability of the catalyst throughout the desorption process are optimized. The TiO₂ shell layer in the Mn₂CoO₄@TiO₂/SO₄²⁻ (MC@TiO₂/S) catalyst effectively inhibits the leaching of active species into the solution, thereby enabling sustained high activity over ten cycles of absorption–desorption testing. The anchoring of protonated groups (SO₄²⁻) facilitates a novel pathway for proton transfer in solution via proton‐coupled electron transfer (PCET) effect, significantly reducing activation energy for this step and enhancing desorption reaction kinetics. Consequently, CO₂ regeneration capacity and regeneration rate increase by 103% and 111%, respectively, while energy consumption during regeneration decreases by ≈44%. Additionally, the environmental performance of the catalyst is evaluated using life cycle assessment (LCA), highlighting its sustainable potential for future scale‐up applications. This study presents a viable strategy for employing metal oxide solid acid materials to facilitate efficient and low‐energy solvent regeneration in carbon capture processes.