Jian Shen

Ag–Cu metal aerogels exhibiting exceptional electrocatalytic properties were synthesized via micro-turbulence, promoting their distinctive 3D architecture formation through a nonclassical growth mechanism.

Amidst global imperatives for sustainable energy and environmental remediation, carbon aerogels (CAs) present a transformative alternative to conventional carbon materials (e.g., activated carbon, carbon fibers), overcoming limitations of disordered pore structures, unmodifiable surface chemistry, and functional inflexibility. This review systematically examines CA-based electrochemical systems as its primary focus, analyzing fundamental charge-storage mechanisms and establishing structure–property–application relationships critical to energy storage performance. We critically assess synthesis methodologies, emphasizing how stage-specific parameters govern structural/functional traits, and detail multifunctional modification strategies (e.g., heteroatom doping, composite engineering) that enhance electrochemical behavior through pore architecture optimization, surface chemistry tuning, and charge-transfer kinetics acceleration. Electrochemical applications are extensively explored, including the following: 1. Energy storage: supercapacitors (dual EDLC/pseudocapacitive mechanisms) and battery hybrids. 2. Electrocatalysis: HER, OER, ORR, and CO₂ reduction reaction (CO₂RR). 3. Electrochemical processing: capacitive deionization (CDI) and electrosorption. Beyond this core scope, we briefly acknowledge CA versatility in ancillary domains: environmental remediation (heavy metal removal, oil/water separation), flame retardancy, microwave absorption, and CO₂ capture.

Halocarbons have important industrial applications, but because of their contribution to global warming and the fact that they can cause ozone depletion, they are considered highly toxic. Hence, the techniques that can capture and recover the used halocarbons with energy‐efficient methods have been recently received greater attention. In this contribution, we report the capture of dichlorodifluoromethane (R12), which has high global warming and ozone depletion potential, using covalent organic polymers (COPs). The defect‐engineered COPs were synthesized and demonstrated outstanding sorption capacities, ~226 wt % of R12 combined with linear‐shaped adsorption isotherms. We further identified the plausible microscopic adsorption mechanism of the investigated COPs via grand canonical Monte Carlo simulations applied to non‐defective and a collection of atomistic models of the defective COPs. The modeling work suggests that significant R12 adsorption performance is attributed to a gradual increment of porosities due to isolated/interconnected micro‐/meso‐pore channels and the change of the long‐range ordering of both COPs. The successive hierarchical‐pore‐filling mechanism promotes R12 molecular adsorption via moderate van der Waals adsorbate‐adsorbent interactions in the micropores of both COPs at low pressure followed by adsorbate‐adsorbate interactions in the extra‐voids created at moderate to high pressure ranges. This continuous pore‐filling mechanism makes defective COPs as promising sorbents for halocarbon adsorption.

This work reports an efficient method for facile synthesis of hierarchically porous carbon (WB‐AC) utilizing wheat bran waste. Obtained carbon showed 2.47 mmol g⁻¹ CO₂ capture capacity with good CO₂/N₂ selectivity and 27.35 to 29.90 kJ mol⁻¹ isosteric heat of adsorption. Rapid removal of MO dye was observed with a capacity of ~555 mg g⁻¹. Moreover, WB‐AC demonstrated a good OER activity with 0.35 V low overpotential at 5 mA cm⁻² and a Tafel slope of 115 mV dec⁻¹. It also exhibited high electrocatalytic HER activity with 57 mV overpotential at 10 mA cm⁻² and a Tafel slope of 82.6 mV dec⁻¹. The large SSA (757 m² g⁻¹) and total pore volume (0.3696 cm³ g⁻¹) result from N₂ activation contributing to selective CO₂ uptake, high and rapid dye removal capacity and superior electrochemical activity (OER/HER), suggesting the use of WB‐AC as cost effective adsorbent and metal free electrocatalyst.

Fenton‐like reaction has been widely used for organics degradation. However, most Fenton‐like reaction works at low pH range (pH < 4) with uncontrollable selectivity of hydroxyl radicals from H₂O₂ activation, and unsatisfied catalyst stability, which is compromised advanced oxidation performance for water/wastewater treatments. In this work, to solve the drawbacks, novel copper catalysts were fabricated via hydrogen reduction/calcination of Cu²⁺‐supported Al/MCM‐41 with precisely controllable copper valence state. Compared with catalysts with monovalence copper (i.e., CuO, Cu, and Cu²⁺), the obtained catalysts with multivalence copper present higher selectivity, excellent stability towards •OH radical pathways, and outperformance in pCBA degradation efficiency at neutral state. In addition, the fabricated catalysts also exhibited excellent phenol removal efficiency (75.5%) and H₂O₂ utilization efficiency (47.9%) within neutral environment. Moreover, the degradation efficiency of phenol approaches to 100% within only 2 h. The catalyst also shows good stability for organic pollutants removal, which shows good potential in catalytic oxidation for phenolic compounds‐containing wastewater in Fenton‐like reaction, especially under neutral pH conditions.Practitioner Points: Multivalence copper presents great potentials for organic compounds removal at neutral condition. Multivalence copper shows higher selectivity toward •OH and good stability at neutral condition. Multivalence copper exhibiters outperformed phenol removal efficiency at neutral condition.