Corvini, Philippe
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Efficient catalytic ozonation over Co-ZFO@Mn-CN for oxalic acid degradation. Synergistic effect of oxygen vacancies and HOO-Mn-NX bonds
2023-03, Xu, Menglu, Zhang, Yibing, Yin, Huaqin, Wang, Jinnan, Li, Aimin, Corvini, Philippe
Hierarchical nano-vesicles with bimetal-encapsulated for peroxymonosulfate activation. Singlet oxygen-dominated oxidation process
2022-04-01, Lyu, Zhiping, Xu, Menglu, Wang, Jinnan, Li, Aimin, Corvini, Philippe
Hierarchical nano-vesicles with bimetal-encapsulated (FeCu1.5O3@NV) was designed for peroxymonosulfate (PMS) activation with the 1O2-dominated oxidation process. Different from previous core–shell metal-loaded catalysts, FeCu1.5O3 was encapsulated in hollow zeolite spheres, and these zeolite sphere units assembled to construct hierarchical nano-vesicles. Owning to mesoporous shell and abundant interior cavity, FeCu1.5O3@NV could enrich reactants in cavity for enhancing the contact with active sites. The flexible surface of bimetal oxides strengthened the affinity with surface adsorbates and substrates, accelerating the electron transfer between reactants. DFT calculation indicated that FeCu1.5O3@NV possessed strong binding affinity for BPA and PMS, facilitating PMS activation and BPA degradation inside of hollow sphere units. Being attributed to the synergistic effect of bimetal redox couples and hierarchical nano-vesicle structure, large amounts of 1O2 could be generated through two pathways for BPA degradation. The first pathway is the reaction between bimetal redox couples and PMS, and the second is the chain reaction of O2•−. Due to bimetal oxides uniformly encapsulated in hierarchical nano-vesicles, FeCu1.5O3@NV possessed high catalytic stability with negligible metal leaching. Even after 5 cycles, BPA removal could still remain 100%.
Engineering efficient hole transport layer Ferrihydrite-MXene on BiVO4 photoanodes for photoelectrochemical water splitting: Work function and conductivity regulated
2022, Bai, Weihao, Zhou, Ye, Peng, Gang, Wang, Jinnan, Li, Aimin, Corvini, Philippe
Although great interest is focused on development of semiconductor photoanodes for efficient photoelectrochemical (PEC) water splitting, the pressing bottleneck to address the intrinsic charge transport for enhancement of PEC performance still remains to be resolved. Herein, hole transport layer (Fh-MXene) constructed by doping of MXene (Ti3C2) in Ferrihydrite (Fh) is loaded on BiVO4 photoanode. This novel BiVO4@Fh-MXene photoanode achieves high current density of 4.55 mA cm−2 at 1.23 V versus reversible hydrogen electrode (vs. RHE), exhibiting excellent photostability. From electrochemical analysis and density functional theory calculations, high PEC performance is ascribed to incorporation of Fh-MXene as hole transport layer, enhancing conductivity and water oxidation reaction. Notably, MXene can improve band alignment of BiVO4/Fh-MXene interface by tuning work function, which strengthens the built-in electric field for more efficient hole extraction. This work provides a simple method to design photoanodes with efficient charge transport layers for feasible PEC water splitting application.
Boosting light harvesting and charge separation over hollow double-shelled Ag@SrTiO3-TiO2 with Z-scheme heterostructure for highly efficient photocatalytic reduction of nitrate to N2
2023-02-01, Zhang, Yixuan, Liu, Cong, Zhou, Ye, Wang, Jinnan, Li, Aimin, Corvini, Philippe
BiOBr/ Bi4O5Br2/PDI constructed for visible-light degradation of endocrine disrupting chemicals. Synergistic effects of bi-heterojunction and oxygen evolution
2022-04-01, Wang, Haoyi, Zhou, Ye, Wang, Jinnan, Li, Aimin, Corvini, Philippe
To remove endocrine disrupting chemicals (EDCs), visible-light response photocatalyst BiOBr/Bi4O5Br2/perylene diimide (PDI) with bi-heterojunction was constructed. Under visible-light irradiation, BiOBr/Bi4O5Br2/PDI could degrade 90% Bisphenol A (BPA) within 75 min, while degrade 100% 17α-ethynyl estradiol (EE2) and 17β-estradiol (E2) within 15 min. Radicals quenching experiment and EPR indicated both •O2– and holes were the main substances for EDCs degradation, and the possible degradation pathway of EDCs are proposed based on the LC-MS analysis results. In the composite of BiOBr/Bi4O5Br2/PDI, the matching energy band structure between Bi4O5Br2 and BiOBr facilitated the formation of heterojunction for strengthening the space charge separation. Meanwhile, PDI with strong photosensitivity combined with BiOBr/Bi4O5Br2 not only enhanced visible-light photocatalytic activity but also broadened the light-harvesting range. Owning to the unique one-dimensional conjugated structure and internal electric field effect, PDI could also promote the photo-carriers transfer and separation. With the bi-heterojunction effect, photo-generated electrons were transferred to BiOBr conduction band while holes were accumulated on PDI valence band. Simultaneously, holes could oxidize water with the production of oxygen following being reduced to •O2– by photo-generated electrons. Even under oxygen-poor conditions, the production of •O2– can reach 32.7 × 10-5mol•g−1•h−1, resulting in more than 85% BPA degradation within 75 min.
Au@CoS-BiVO4 {010} constructed for visible-light-assisted peroxymonosulfate activation
2021-11-22, Ji, Yekun, Zhou, Ye, Wang, Jinnan, Li, Aimin, Bian, Weilin, Corvini, Philippe
A visible-light-Fenton-like reaction system was constructed for the selective conversion of peroxymonosulfate to sulfate radical. Au@CoS, when doped on monoclinic BiVO4 {010} facets, promoted spatial charge separation due to the different energy band between the m-BiVO4 {010} and {110} facets. The visible-light response of m-BiVO4 was enhanced, which was attributed to the SPR effect of Au. And the photogenerated electrons were transferred from the m-BiVO4 {010} facet to Au via a Schottky junction. Owing to higher work function, CoS was able to capture these photoelectrons with acceleration of the Co(Ⅱ)/Co(Ⅲ) redox, enhancing peroxymonosulfate conversion to sulfate radical (Co2+ + HSO5−→ Co3+ + •SO4− + OH−). On the other hand, holes accumulated on m-BiVO4 {110} facets also contributed to organics oxidation. Thus, more than 95% of RhB was degraded within 40 min, and, even after five cycles, over 80% of RhB could be removed. The radical trapping experiments and EPR confirmed that both the sulfate radical and photogenerated hole were the main species for organics degradation. UV-vis DRS, photoluminescence (PL) and photoelectrochemical analyses also confirmed the enhancement of the visible-light response and charge separation. In a pilot scale experiment (PMS = 3 mM, initial TOC = 151 mg/L, reaction time = 4 h), CoS-Au-BiVO4 loaded on glass fiber showed a high mineralization rate (>60%) of practical wastewater.
Assessing the biodegradation of btex and stress response in a bio-permeable reactive barrier using compound-specific isotope analysis
2022-07-20, Chen, Tianyu, Wu, Yan, Wang, Jinnan, Corvini, Philippe
By using compound-specific isotope analysis (CSIA) in combination with high-throughput sequencing analysis (HTS), we successfully evaluated the benzene and toluene biodegradation in a bio-permeable reactive barrier (bio-PRB) and the stress response of the microbial community. Under stress conditions, a greater decline in the biodegradation rate of BTEX was observed compared with the apparent removal rate. Both an increase in the influent concentration and the addition of trichloroethylene (TCE) inhibited benzene biodegradation, while toluene biodegradation was inhibited by TCE. Regarding the stress response, the relative abundance of the dominant bacterial community responsible for the biodegradation of BTEX increased with the influent concentration. However, the dominant bacterial community did not change, and its relative abundance was restored after the influent concentration decreased. On the contrary, the addition of TCE significantly changed the bacterial community, with Aminicenantes becoming the dominant phyla for co-metabolizing TCE and BTEX. Thus, TCE had a more significant influence on the bio-PRB than an increasing influent concentration, although these two stress conditions showed a similar degree of influence on the apparent removal rate of benzene and toluene. The present work not only provides a new method for accurately evaluating the biodegradation performance and microbial community in a bio-PRB, but also expands the application of compound-specific isotope analysis in the biological treatment of wastewater.
Ultrafine-Mn2O3@N-doped porous carbon hybrids derived from Mn-MOFs: Dual-reaction centre catalyst with singlet oxygen-dominant oxidation process
2022, Xie, Zhiqun, Lyu, Zhiping, Wang, Jinnan, Li, Aimin, Corvini, Philippe
Ultrafine-Mn2O3@N-doped porous carbon hybrids [Mn2O3@NC] derived from Mn-MOFs was constructed with 1O2 and O2−• as main Reactive oxygen species (ROS). Cation-π bonds and N-Mn complexation induced the formation of electron-rich Mn centre which provided electron for peroxymonosulfate activation to produce radicals, accompanying with generation of 1O2 via chain reaction. Notably, the porous structure of N-doped carbon shell could not only facilitate free radical recombination for generation of 1O2 but also provide adsorption sites for organics. On the other hand, as electron-poor centre, N-doped carbon shell could improve the electrons transfer from organic intermediate radicals to electron-rich Mn centre via π -π reaction, C-O-Mn and C-N-Mn bonds, which promote the redox of Mn to avoid peroxymonosulfate invalid decomposition. Being attributed to synergistic effects of dual-reaction centres and strong oxidation ability of 1O2, Mn2O3@NC achieved high mineralization of BPA at low-dose peroxymonosulfate (0.033 g/L).