Morphology–Coordination Coupling of Fe–TCPP and g-C3N4 Nanotubes for Enhanced ROS Generation and Visible-Light Photocatalysis

Abstract

Fe–porphyrin/g-C3N4 composites have emerged as promising visible-light photocatalysts, but their performance remains limited by inefficient charge separation and low reactive oxygen species (ROS) yield. Here, iron–tetra(4-carboxyphenyl) porphyrin (Fe–TCPP) was coupled with g-C3N4 nanotubes (CNNTs) via a facile self-assembly strategy, creating a morphology-coordinated system. Comprehensive characterization (XRD, FTIR, SEM/TEM, BET, UV–Vis diffuse reflectance, PL, XPS, and EPR) confirmed the structural integrity, electronic coupling, and ROS generation capability of the composites. Fe–TCPP incorporation narrowed the bandgap from 2.78 to 2.56 eV, prolonged the average carrier lifetime from 6.3 to 7.5 ns, and significantly enhanced the generation of •OH and 1O2. The optimized 1 wt% Fe–TCPP@CNNTs achieved complete Rhodamine B degradation within 30 min under visible light, with the highest two-stage apparent rate constants (k1 = 0.0964 min−1, k2 = 0.328 min−1). In addition, the hybrids retained over 90% activity after six consecutive runs, confirming their stability and recyclability. The synergistic effect of Fe–N coordination and nanotubular architecture thus promotes light harvesting, charge separation, and ROS utilization, offering a promising design principle for high-performance photocatalysts in environmental remediation.