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APPLIED CATALYSIS B-ENVIRONMENTAL · 2019 · IF 14.229

Coordinate activation in heterogeneous carbon dioxide reduction on Co-based molecular catalysts

Xiangdong Kong,Yan Liu,Pai Li,Jingwen Ke,Zhongyu Liu,Fawad Ahmad,Wensheng Yan,Zhenyu Li,Zhigang Geng,Jie Zeng

As CO 2 coordination with the metal sites in molecular catalysts represents an effective means to CO 2 activation, it is important to develop molecular catalysts with high ability of CO 2 coordination to enhance their catalytic performance in CO 2 electroreduction. Herein, we investigated the coordinate activation of CO 2 with Co-based molecular catalysts by manipulating their ligand structures. During CO 2 electroreduction, the current density of Co-salophen for CO was −16.0 mA cm −2 at −0.75 V versus reversible hydrogen electrode ( vs RHE), which was 7.6 times of that (−2.1 mA cm −2 ) of Co-salen. In addition, the Faradaic efficiency (FE) of Co-salophen for CO reached 75 % at −0.70 V vs RHE, whereas the FE of Co-salen for CO production was 19 %. In-situ experiments and mechanistic studies revealed that both Co-salophen and Co-salen adopted a side-on coordination of CO 2 with Co sites. Moreover, the bonding between CO 2 and Co sites was strengthened in Co-salophen, resulting in the enhanced activity of Co-salophen.

研究领域: 化学 · 催化科学
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APPLIED CATALYSIS A-GENERAL · 2023 · IF 5.5

Improving photocatalytic degradation of enrofloxacin over TiO2 nanosheets with Ti3+ sites by coordination activation

Jiayang Zheng,Cheng Liu,Zhiwen Wang,Yingzhang Shi,Yidong Hou,Jinhong Bi,Ling Wu

Ultrathin TiO 2 nanosheets (NST) containing Ti 3+ sites are developed as a photocatalyst that exhibits high degradation efficiencies (98.6%) for the degradation of enrofloxacin (ENR) under visible light. The increment of degradation efficiencies for ENR over NST is mainly due to the increase of Ti 3+ and oxygen vacancies (OVs). Ti 3+ sites on the surface of NST can be associated with ENR molecules through the formation of surface coordination species -COO∙∙∙Ti- intermediates, resulting in the activation of ENR. OVs on NST can adsorb and activate more O 2 molecules to accelerate the generation of O 2 - by photogenerated electrons reduction. The photogenerated holes quickly transfer to the surface of the catalyst to directly degrade the activated ENR. Finally, a possible mechanism about the synergistic effect of coordination activation and photocatalysis is proposed over NST at a molecule level. This study highlights the significant role of coordination activation in the photocatalytic degradation of antibiotics.

CAS / MDL: 111-40-0 546-68-9
研究领域: 环境科学 · 材料科学 · 化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Ultrathin 2D/2D MoS2/Bi2WO6 S-scheme heterojunction for boosting photocatalytic degradation of ciprofloxacin

Qi Chen,Cheng Liu,Rui Liu,Yidong Hou,Jinhong Bi,Jimmy C. Yu,Ling Wu

A series of 2D/2D MoS 2 /Bi 2 WO 6 S-scheme heterojunctions consisting of ultrathin MoS 2 nanosheets (MS, 1.6 nm) and ultrathin Bi 2 WO 6 nanosheets (BWO, 1.5 nm) were developed for photocatalytic degradation of ciprofloxacin. The samples with 5 % mass ratio of MS (5 %MS/BWO) exhibits the almost complete degradation of ciprofloxacin (≈100 %) under visible light. It is evidenced that the formation of S-scheme heterojunction with close interfacial interaction facilitates the photoinduced carrier separation and the generation of surface acid sites. The activation of ciprofloxacin molecules is realized through the coordinately interaction of C-N and C=O with the surface W sites. Moreover, the OVs in BWO side is a convenient pathway for activated of O 2 , embodying in the generation of •O 2 − and •OH under visible light over photocatalyst. Such an association of charge transfer mechanism with coordination activation shows the enhanced photocatalytic performance toward ciprofloxacin. This work provides a motivation which designs an S-scheme heterojunction photocatalyst with the ability to activate the specific group in molecules to comprehend the degradation of antibiotics.

CAS / MDL: 85721-33-1 57-09-0
研究领域: 材料科学 · 环境科学 · 化学
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CHEMOSPHERE · 2024 · IF 8.1

Cu2O/WO3 S-scheme heterojunctions for photocatalytic degradation of levofloxacin based on coordination activation

Qi Chen,Ling Hu,Yingzhang Shi,Cheng Liu,Yidong Hou,Jinhong Bi,Jimmy C. Yu,Ling Wu

Heterogeneous photocatalytic degradation of antibiotic involves the activation of antibiotic molecules and the photocatalytic oxidation process. However, the simultaneous improvement of these processes is still a challenge. Herein, S-scheme heterojunctions consisted of Cu 2 O nanocluster with defective WO 3 nanosheets were constructed for efficient photocatalytic degradation of levofloxacin (LVX). The typical CNS-5 composite (5 wt% Cu 2 O/WO 3 ) achieves an optimal LVX degradation efficiency of 97.9% within 80 min. The spatial charge separation and enhancement of redox capacity were realized by the formation of S-scheme heterojunction between Cu 2 O and WO 3 . Moreover, their interfacial interaction would lead to the loss of lattice oxygen and the generation of W 5+ sites. It is witnessed that the C–N of piperazine ring and C O of carboxylic acid in LVX are coordinated with W 5+ sites to build the electronic bridge to activate LVX, greatly promoting the further degradation. This work highlights the important role of selective coordination activation cooperated with S-type heterojunctions for the photocatalytic degradation and offers a new view to understand the degradation of antibiotics at molecular level.

研究领域: 环境科学 · 材料科学 · 化学
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Journal of Environmental Chemical Engineering · 2022 · IF 7.968

Coordination activation enhanced photocatalytic performance for levofloxacin degradation over defect-rich WO3 nanosheets

Ling Hu,Zhiwen Wang,Yingzhang Shi,Cheng Liu,Yidong Hou,Jinhong Bi,Ling Wu

The defect-rich ultrathin WO 3 nanosheets are successfully prepared as photocatalysts via heating treatment for the pristine WO 3 nanosheets (NS) in vacuum (NSV) and N 2 atmosphere (NSN). The increment of degradation efficiencies of levofloxacin (LVX) over NS (49.9 %)

CAS / MDL: 100986-85-4
研究领域: 环境科学 · 材料科学 · 化学
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