Corvini, Philippe
Lade...
E-Mail-Adresse
Geburtsdatum
Projekt
Organisationseinheiten
Berufsbeschreibung
Nachname
Corvini
Vorname
Philippe
Name
Corvini, Philippe
67 Ergebnisse
Suchergebnisse
Gerade angezeigt 1 - 10 von 67
Publikation Electrochemical reconfiguration of NiFe layered double hydroxide on BiVO4 induced by black phosphorus quantum dots for promoting photoelectrochemical water splitting(Elsevier, 12/2024) Sun, Yunshuyu; Chen, Hao; Hou, Zhiang; Wang, Jinnan; Li, Aimin; Corvini, PhilippeIn this work, black phosphorus quantum dots (BPQDs) and NiFe layered double hydroxide (NiFe-LDHs) were loaded on BiVO4 photoanode for promoting photoelectrochemical (PEC) water splitting. As a narrow bandgap p-type semiconductor with high work function, BPQDs could not only form p-n junction with BiVO4 to enhance light harvest but also construct Schottky junction for charge carriers separation. More importantly, introduction of BPQDs facilitates the transformation of Ni(OH)2 into NiOOH so as to improve the water oxidation capacity at low bias voltage. Density functional theory (DFT) calculation demonstrates that introduction of BPQDs accelerates the α/γ phase transition dynamically and thermodynamically, thus BiVO4/BPQDs/NiFe-LDHs photoanode achieves photocurrent density of 5.28 mA cm−2 at 1.23 VRHE, AM 1.5 G and maintains good stability. In summary, this work provides new ideas for constructing efficient hole extraction layers on photoelectrode, well expanding the application of BPQDs in PEC water splitting.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Bi atom sharing Co-Bi₂O₂CO₃/BiOI S-scheme induced singlet oxygen-dominated photocatalytic oxidation system(Elsevier, 12/2024) Hou, Zhiang; Yue, Jinzhu; Chen, Hao; Wang, Jinnan; Li, Aimin; Corvini, PhilippeEndocrine disrupting chemicals (EDCs) interfere with the normal secretion, transport and metabolism of human hormones, thus affecting neurological, reproductive and immune functions. Photocatalysis is regarded as a facile organic degradation technique. The construction of heterojunctions can modulate the reactive oxygen species and enhance the photocatalytic performance of semiconductors. However, poor contact interfaces still severely limit carrier separation and transfer. Herein, we have doped Co to modulate the band structure of Bi₂O₂CO₃ while facilitating the in situ growth of BiOI on its surface via shared Bi atoms. This approach led to the development of a 2D/2D Co-Bi₂O₂CO₃/BiOI (Co-BOC/BiOI) S-scheme heterojunction characterized by atomically close contact interfaces. Furthermore, the photo-electrochemical characterization results indicate that the light adsorption capacity, carrier separation and transport efficiency of the optimized Co-BOC/BiOI-3 are greatly improved. This system demonstrates almost 100% removal rate for three typical EDCs within 60 min. The degradation kinetic constants show an improvement by an order of magnitude compared to single BiOI and Bi₂O₂CO₃. More importantly, O₂•﹣, which is produced from O₂ reduction on high negative conduction band, can be subsequently oxidized into 1O2 by photogenerated hole. Electron paramagnetic resonance and quenching experiments indicate that the organics degradation process is dominated by 1O2. This work offers new insights into the construction of high-quality S-scheme heterojunction interfaces for modulation of reactive oxygen species.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Modulating the electronic structure of Mn promotes singlet oxygen generation from electrochemical oxidation of H₂O via O-O coupling(Elsevier, 12/2024) Chen, Hao; Hou, Zhiang; Yue, Jinzhu; Wang, Jinnan; Wang, Yi; Li, Aimin; Corvini, PhilippeSelectively catalytic conversion H₂O into singlet oxygen (¹O₂) without additional oxidants is considered as an economic-efficient method for organic pollutants degradation. However, H₂O are more consistent with the spin state of ¹O₂ than common oxygen (O₂), retarding the kinetics of spin transition-induced reaction between O₂ and ¹O₂. Herein, we report an unprecedented ¹O₂ mediated electrocatalytic oxidation process, which allows O–O coupling for ¹O₂ evolution from H₂O over CrMn@C anode. The electron occupancy (eg) of CrMn@C (0.89) is very close to the optimal eg (0.95) of manganese-based materials reported in the literature, which facilitates the activation of H₂O on surface. Mn(Mn0.193Cr1.808)O₄-Mn in CrMn@C electrode significantly promotes the activation of H₂O to produce *O, followed by coupling of *O at adjacent sites to produce *OO, which further spontaneously forms ¹O₂. And H₂¹⁸O isotope experiments provide direct evidence for the production of ¹O₂ directly from H₂O. Consequently, the production of ¹O₂ is enhanced with the yield of 785.6 μmol·L⁻¹. Such ¹O₂-dominated electrocatalytic oxidation system can achieve efficient removal of electron-rich pollutant (bisphenol A) and improve the biodegradability of pharmaceutical wastewater (from 0.17 to 0.39).01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Phosphorization of α-Fe₂O₃ boosts active hydrogen mediated electrochemical nitrate reduction to ammonia(Wiley, 25.09.2024) Hou, Zhiang; Zhang, Yixuan; Chen, Hao; Wang, Jinnan; Li, Aimin; Corvini, PhilippeInexpensive iron-based materials are considered promising electrocatalysts for nitrate (NO₃−) reduction, but their catalytic activity and spontaneous corrosion remain challenges. Here, the α-Fe₂O₃ active surface is reconstructed by gradient phosphorization to obtain FePₓ with higher electrochemical activity. FeP₂.₀ optimizes the adsorption energy of NO₃- and its reduction intermediates, meanwhile promote the generation of active hydrogen (*H) but inhibit its generation of H₂. More importantly, Fe and P can serve as binding sites for NO₃- and *H, respectively, which improves the electron utilization of NO₃- deoxygenation and the efficiency of the subsequent hydrogenation for the selective synthesis of NH₃. 91.7% NO₃- conversion rate is achieved for the reduction of 100 mL 200 mg L-¹ NO₃−−N, 99.3% ammonia (NH₃ selectivity (yield of 1.79 mg h−¹ cm−2), and 91.4% Faraday efficiency in 3 h. The high-purity solid NH₄Cl is finally extracted by gas extraction and vacuum distillation (81.4% recovery). This study provides new insights and strategies for the conversion of NO₃− to NH₃ products over iron-based electrocatalysts.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Amorphous metal-organic frameworks loaded on BiVO4 photoanodes with unique internal metal-like structure for promoting photoelectrochemical water splitting(Elsevier, 09/2024) Bai, Weihao; Li, Hao; Peng, Gang; Wang, Jinnan; Li, Aimin; Corvini, PhilippeAlthough ferrocene (Fc) based Metal-Organic Frameworks (MOFs) can act as oxygen evolution co-catalysts (OECs) for improvement of catalytic reactivity, the poor conductivity and lack of highly active metal sites limit its further application in photoelectrochemical (PEC) water splitting. Herein, the amorphous NiFc-MOF was grafted on BiVO4 photoanode (BiVO4@aNiFc-MOFs) for efficient PEC water splitting. This novel BiVO4@aNiFc-MOFs exhibits high current density of 4.34 mA cm−2 at 1.23 VRHE and relative low onset potential of 0.223 VRHE. The subsequent characterizations demonstrate that Ni species with metal-like state in bulk of aNiFc-MOFs form strong metal-support interaction with BiVO4, thereby promoting the interfacial charge transfer. Moreover, the surface of aNiFc-MOFs is short-range ordered with abundant coordinatively unsaturated Ni sites, creating a more favorable pathway for oxygen evolution reaction from thermodynamics. This work provides a simple method to design photoanodes with efficient OECs of amorphous MOFs for feasible PEC water splitting application.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Maize (Zea mays L.) plants change their fate and accumulate non-extractable residues of sulfamethoxazole in the soil of arable land(American Chemical Society, 16.05.2024) Wu, Xuan; Sun, Feifei; Cao, Siqi; Wang, Qilin; Wang, Lianhong; Wang, Songfeng; He, Yan; Kolvenbach, Boris; Corvini, Philippe; Ji, RongThe fate of sulfonamide antibiotics in farmlands is crucial for food and ecological safety, yet it remains unclear. We used [phenyl-U-14C]-labeled sulfamethoxazole (14C-SMX) to quantitatively investigate the fate of SMX in a soil–maize system for 60 days, based on a six-pool fate model. Formation of nonextractable residues (NERs) was the predominant fate for SMX in unplanted soil, accompanied by minor mineralization. Notably, maize plants significantly increased SMX dissipation (kinetic constant kd = 0.30 day–1 vs 0.17 day–1), while substantially reducing the NER formation (92% vs 58% of initially applied SMX) and accumulating SMX (40%, mostly bound to roots). Significant NERs (maximal 29–42%) were formed via physicochemical entrapment (determined using silylation), which could partially be released and taken up by maize plants. The NERs consisted of a considerable amount of SMX formed via entrapment (1–8%) and alkali-hydrolyzable covalent bonds (2–12%, possibly amide linkage). Six and 10 transformation products were quantified in soil extracts and NERs, respectively, including products of hydroxyl substitution, deamination, and N-acylation, among which N-lactylated SMX was found for the first time. Our findings reveal the composition and instability of SMX-derived NERs in the soil–plant system and underscore the need to study the long-term impacts of reversible NERs.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Investigation of biologically active zeolite. Role of colonization in the removal of 14C-labelled sulfamethoxazole in wastewater(Elsevier, 02/2024) Cuomo, Maurizio; König, Roger; Zanardini, Elisabetta; Di Guardo, Antonio; Terzaghi, Elisa; Kolvenbach, Boris; Demaria, Francesca; Corvini, Philippe; Principi, PamelaUp-to-date approaches to remove micropollutants in wastewater treatment are based on adsorbing materials like activated carbon. These fossil-based materials can also provide a surface for microbial colonization, which could further improve the removal of MPs. As zeolite filters have shown interesting performance in the removal of MPs in previous works, this study aimed to investigate the effect of microbial colonization on such filters on the elimination of 14C-labelled sulfamethoxazole (SMX), an antibiotic from the class of sulfonamides. Lab scale removal tests were set in 100 mL reactors and monitored for 150 days at room temperature. Taxa known to be linked to organic pollutant degradation (Caulobacterales, Rhizobiales, Burkholderiales) were found among the microbial community attached to the zeolite. Bacterial colonization of zeolite filters improved the removal of 14C-sulfamethoxazole by 35 % compared to the control. An analysis of the microbial community dynamics over time revealed the increased abundance of the Vicinamibacterales taxon after 50 days of contact with SMX. This order abundance, linked to degradation of sulfonamides, went from 0 to 17 %; and Shannon diversity ranged from 1.51 to 1.99. Data showed that zeolite filters as adsorbing material in wastewater treatment plants can improve MPs removal by supporting bacterial colonization, making it an interesting support that could synergize with biological activated carbon.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Pollutant profile complexity governs wastewater removal of recalcitrant pharmaceuticals(Nature, 2024) Suleiman, Marcel; Le Lay, Natalie; Demaria, Francesca; Kolvenbach, Boris; Cretoiu, Mariana; Petchey, Owen; Jousset, Alexandre; Corvini, PhilippeOrganic pollutants are an increasing threat for wildlife and humans. Managing their removal is however complicated by the difficulties in predicting degradation rates. In this work, we demonstrate that the complexity of the pollutant profile, the set of co-existing contaminants, is a major driver of biodegradation in wastewater. We built representative assemblages out of one to five common pharmaceuticals (caffeine, atenolol, paracetamol, ibuprofen, and enalapril) selected along a gradient of biodegradability. We followed their individual removal by wastewater microbial communities. The presence of multichemical background pollution was essential for the removal of recalcitrant molecules such as ibuprofen. High-order interactions between multiple pollutants drove removal efficiency. We explain these interactions by shifts in the microbiome, with degradable molecules such as paracetamol enriching species and pathways involved in the removal of several organic pollutants. We conclude that pollutants should be treated as part of a complex system, with emerging pollutants potentially showing cascading effects and offering leverage to promote bioremediation.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Circularity and environmental sustainability of organic and printed electronics(Jenny Stanford Publishing, 2024) Le Blévennec, Kévin; Hengevoss, Dirk; Zimmermann, Yannick-Serge; Brun, Nadja; Hugi, Christoph; Lenz, Markus; Corvini, Philippe; Fent, Karl; Nisato, Giovanni; Lupo, Donald; Rudolf, SimoneIn this chapter, the possible role and impact of organic and printed electronics (OPE) in a transition toward a circular economy and more sustainable society will be discussed. The learning targets are twofold: first, understanding main environmental issues associated with the emerging field of OPE, and second, identifying, through a systemic perspective, the enabling potential of these technologies.04A - Beitrag SammelbandPublikation Single-atomic ruthenium coupling with NiFe layered double hydroxide in-situ growth on BiVO₄ photoanode for boosting photoelectrochemical water splitting(Elsevier, 01/2024) Sun, Yunshuyu; Li, Hao; Hu, Yao; Wang, Jinnan; Li, Aimin; Corvini, PhilippeIn the present work, NiFe layered double hydroxide (LDH) supported single Ru atoms in-situ growth on BiVO₄ photoanode (BiVO₄@NiFe-LDHs/Ru) was fabricated to enhance the photoelectrochemical (PEC) water splitting. Ru atoms anchored to NiFe-LDHs via oxygen coordination to form Ru-O-M bonds, which induced electrons rearrangement to improve charge carriers separation and injection. Combining with the synergistic effect of Ru and NiFe-LDHs, BiVO₄@NiFe-LDHs/Ru achieves high photocurrent density of 4.65 mA/cm² at 1.23 V vs. RHE. Besides, Ru atoms induced formation of V⁽⁵⁻ˣ⁾⁺ to stabilize V atoms in the lattice of BiVO4, which avoided V5+ dissolution during PEC water oxidation process. Density functional theory (DFT) calculation indicates that Ru SAs anchored to BiVO₄@NiFe-LDHs decrease the reaction energy barrier of rate-limiting step (*O → *OOH), resulting in acceleration of OER process. This work provides an effective pathway to design high efficient and stable photoanodes with single atoms for feasible PEC water splitting application.01A - Beitrag in wissenschaftlicher Zeitschrift