Faculty of Humanities and Sciences
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Publication Open Access Coconut Shell Waste-Derived Porous Carbon-Supported Sn Catalysts for Efficient Electrochemical CO2Reduction to Formic Acid and Deuterated Formic Acid(American Chemical Society, 2025-11-05) Qin, C; Masakorala, G; Mohideen, M; Samarasekara, T; Zhang, L; Zhu, W; Zhou, Y; Thambiliyagodage, CIndustrial-level electrochemical CO2 reduction reaction (CO2RR) to form HCOO– and DCOO– requires robust Sn catalysts with high performance. In this study, the hydrothermal method was employed to load varying amounts of Sn precursors onto waste biomass-derived porous carbon to investigate the structure–activity relationship between Sn loading forms and HCOO– selectivity. Through comprehensive ex/in situ characterizations, we discovered that with 5% Sn precursor addition, highly dispersed SnO2 nanoparticles formed on the carbon support, enabling the catalyst to exhibit exceptional HCOO– activity (Faradaic efficiency exceeding 90%) across a broad potential window. In situ attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR) and in situ Raman spectroscopy revealed that the highly dispersed SnO2 nanoparticles enhance the stability of the *OCHO intermediate. Furthermore, when H2O was replaced with D2O, the generation of DCOO– was observed, and good selectivity was maintained. This study provides a facile strategy for waste biomass conversion and the design of Sn-based catalysts for DCOO– production.Publication Open Access ZIF-8 confined carbon dots/bilirubin oxidase on microalgal cells to boost oxygen reduction reaction in photo-biocatalytic fuel cells for pollutants removal(Elsevier B.V., 2026-01) Qing, S; Lu, X; Jiang, Y; Thambiliyagodage, C; Song, B; Xia, A; Zhang, J.R; Zhu, W; Jiang, L.P; Wu, XPhotocatalytic fuel cells provide promising opportunities for sustainable wastewater treatment and energy conversion. However, their applications are challenged by the sluggish oxygen reducton reaction (ORR) kinetics at cathodes owning to the low O2 solubility and diffusion rate. Herein, we proposed a photo-biocatalytic fuel cell (PBFC) with a novel hybrid biocathode based on artificially engineered algal cells coated by ZIF-8 confined carbon dots/bilirubin oxidase (ZIF-8/CDs/BOD@algae). Microalgae absorbed CO2 and provided O2 in situ for BOD catalysts. Due to effective absorption of O2 by imidazole and confinement of hydrophobic porous ZIF-8, oxygen diffusion has been accelerated in MOF/enzyme systems. Importantly, the introduction of CDs alleviated the poor conductivity of ZIF-8 and improved the electron transfer rate of BOD. Thus, the biocathode exhibited a high current density of 1767 μA/cm2, a 2.26-fold increase compared with that of CDs/BOD/algae biocathode. Also, it displayed enduring operational stability for up to 60 h since the firmly wrapped ZIF-8 shells could encapsulate proteins and protect algae from the external stimulation. When coupled with Mo:BiVO4 photoanodes, the PBFC exhibited a remarkable power output of 131.8 μW/cm2 using tetracycline hydrochloride (TCH) as a fuel and an increased degradation rate of TCH. Therefore, this work not only establishs an effective confinement strategy for enzyme to enrich oxygen, but also unveils new possibilities for modified microalgal cells aiding photoelectrocatalytic systems to recover energy from wastewater treatment.Publication Embargo Heterojunction and homojunction engineering on multi-shelled confinement structure for CO2 photoreduction to CH4(Elsevier B.V., 2025-10-15) Yang, X; Yang, R; Lu, X; Cao, Y; Ye, P; Zhang, L; Li, K; Li, Z; Jiang, Y; Liu, J; Zhou, Y; Eroglu, Z; Thambiliyagodage, C; Wu, B; Metin, Ö; Zhou, Y; Zhu, WThe underdeveloped CO2 photo-reduction solid-gas mode still relies on precious metals to produce CH4. Fine-tuned ingenious structure and morphology with nonprecious metal can enable better performance with lower cost. We have synthesized and modified a TiO2 with a three-stage cavity and a three-shelled layer, loaded with In2S3 flakes only on the outermost layer. The porous hollow multi-shelled structure can give a sequence of gas diffusion from inside to outside or vice versa. Due to the confinement effect, products generated by the core can only be transferred from the inside to the outside in a unidirectional manner. The In2S3/TiO2 catalysts exhibited high performance comparable to that of conventional noble metal catalysts (e.g., Au-Ag-Pt), with a selectivity of up to 98.28 % for CH4 and a rate of 296.87 μmol·g−1·h−1 without using any co-catalyst or sacrificial agent. Systematic fundamental characterization, as well as in situ characterization and DFT calculations show that homo-junctions consisting of two crystalline phases of TiO2 contribute to the production of more *Hads and *CO. Desorbed CO can be captured and catalyzed by the outer shell In2S3/TiO2 S-scheme heterojunction during diffusion for methanation via formaldehyde intermediate. A series of photoelectrochemical characterizations also confirms that the In2S3/TiO2 hetero-junction improves light absorption and charge separation efficiency. This work provides insight into the future rational design of hollow semiconductors for artificial photosynthesis systems and selective solar fuel production.
