Jianming Pan

Pseudocapacitive electrode-based capacitive deionization (CDI) is a competitive water purification technology, yet organic electrodes are limited by insufficient redox activity and sluggish adsorption kinetics in practical use. A novel sulfur-bridged polymer (SPTCDA) was developed as the electrode for a hybrid CDI (HCDI) system to address efficient ammonium ion (NH4+) removal and recovery from industrial wastewater. Experimental characterizations and density functional theory calculations confirm that SPTCDA’s ladder-type conjugated structure, delocalized π-electron system, and structural flexibility synergistically boost conductivity, ion diffusion, and NH4+ affinity. The SPTCDA-HCDI system achieves a high NH4+ capacity of 190.87 mg g–1 at 1.6 V, a fast deammoniation rate (>18 mg g–1 min–1), low energy consumption (<60 kJ mol–1), and 91.5% capacity retention after 100 cycles. It also enables simultaneous removal of dyes and antibiotics, with the recovered ammonium solution reusable for irrigation. This sulfur-bridged polymer design provides a scalable route for high-performance electrochemical water treatment.

Selective enrichment of Ga(III) from acidic zinc hydrometallurgical solutions remains challenging because of the low Ga(III) concentration and the coexistence of competing metal ions. Herein, an ester-containing conjugated microporous polymer, CMP-mCOOCH3, was used as a precursor to construct hydroxamic acid-functionalized CMP-mCONHOH and carboxyl-functionalized CMP-mCOOH through postsynthetic modification. This design enables a direct comparison of how different O-donor coordination environments regulate Ga(III) adsorption within a similar porous framework. Both materials showed efficient Ga(III) uptake at pH 3 and 298 K, with adsorption capacities of 174.75 mg g–1 for CMP-mCONHOH and 249.47 mg g–1 for CMP-mCOOH. The adsorption processes followed pseudo-second-order kinetics and Langmuir isotherm behavior, indicating coordination-driven monolayer adsorption. In competitive systems, both adsorbents maintained good Ga(III) uptake in the presence of Al(III), Zn(II), and Cu(II), whereas In(III) showed stronger competition. CMP-mCOOH exhibited a higher adsorption capacity, while CMP-mCONHOH showed stronger chelation-driven recognition, especially for Ga/In separation. After five adsorption–desorption cycles, CMP-mCONHOH and CMP-mCOOH retained 90.4% and 92.2% of their adsorption efficiencies, respectively. Spectroscopic analyses and theoretical calculations revealed that Ga(III) binding mainly occurred through oxygen-donor coordination. These results provide guidance for designing regenerable porous polymer adsorbents for gallium recovery from acidic metallurgical systems.

The energy‐free activation of ambient molecular oxygen (O ₂ ) to singlet oxygen ( ¹ O ₂ ) under neutral conditions is highly desirable for green oxidation chemistry, yet remains fundamentally limited by sluggish proton‐coupled *OOH formation and desorption. Here, we engineer an interfacial proton‐relay microenvironment between MoS ₂ and CuCl that enables self‐driven O ₂ ‐to‐ ¹ O ₂ conversion without external energy inputs. Electron‐deficient sulfur sites act as a proton reservoir by forming S‐H _ads species, facilitating directional proton migration through Cu‐S‐Mo channels to activate adsorbed O ₂ on electron‐rich Cu sites. This coupled electron‐proton relay accelerates *OOH hydrogenation while maintaining moderate *O2/*OOH binding, effectively suppressing O─O bond cleavage and favoring a 1O2‐dominated pathway. As a result, the system achieves quantitative pollutant removal and sustained operation for over 16 h in pilot‐scale membrane filtration. This interfacial design is broadly applicable to transition metal sulfides, offering a general strategy to overcome proton‐transfer limitations and advance autonomous catalytic platforms for sustainable oxidation and environmental remediation.

Two Au(III) tetrapyrrole complexes were obtained from the reaction of a bent-shaped benzohomoporphyrin ligand and Au(III) acetate. Despite the small size of the tetrapyrrolic ligands, the Au(III) complexes exhibited a low-energy NIR absorption. Combined density functional theory and TDDFT calculations with natural transition orbital (NTO) (NTO) analysis show that the NIR absorption is dominated by intraligand π → π* excitations with only minor Au-centered acceptor mixing rather than by ligand-to-metal charge transfer. The NIR absorption is therefore attributed to a resonance- and structure-controlled narrowing of the frontier orbital gap within the non-aromatic benzohomoporphyrin framework. The generation of O₂^•– by gold complexes was investigated upon photoirradiation, and both Au(III) tetrapyrrole complexes showed high O₂^•– generation efficiency.

Pyrrole appending converts the peripheral site of an N-confused porphyrin into a robust monoanionic N,N chelate, enabling stable mono- and bis-Rh(I) complexes with square-planar Rh-N₂(CO)₂ environments. Both complexes show broad visible-NIR absorption and dual photodynamic-photothermal activity. Mono-Rh(I) 3-Rh exhibits higher singlet-oxygen yields under green and 808 nm excitation, whereas bis-Rh(I) 3-Rh₂ displays superior photothermal efficiency. Computations reveal ligand-centered excitations in 3-Rh and enhanced metal-ligand mixing in 3-Rh₂, explaining their distinct energy-dissipation pathways.

Dual N/Se-doped resorcinol-formaldehyde microspheres (Se-RF) were developed for efficient Pd recovery. The N moieties, derived from ammonia act as “protonated dispersive bait”, while Se centers act as “specific anchoring sites” for Pd( ii ).

Herein, we present a regiodivergent method for N1- and C3-alkylation of indoles with reversed polarity, triggered by the incorporation of a benzoyloxy leaving group at the N1-position. This approach employs Grignard reagents as versatile nucleophiles, in contrast to conventional regiodivergent indole alkylation methods that rely on alkenes as alkylation reagents. The key to achieving switchable regioselectivity is our discovery that cyclic ether solvents can suppress background N1-alkylation, allowing copper catalysis to selectively divert reactivity toward the C3-position. This reaction system exhibits complete conversion, nearly absolute regioselectivity, and excellent yields across a broad scope of Grignard reagents and substrates.