Surfaces and Interfaces
·
2021
·
IF 4.837
Chunli Wang,Yunxiang Dai,Xiaoheng Fu,Hongbo Lu,Jing Zhang
In this work, a novel 2-dimentional (2D)-2D bentonite/g-C 3 N 4 composite (B/g-C 3 N 4 ), with a layer-layer cross structure and large surface area, was synthesized by a self-assembly process, with the aim for the photocatalytic oxidation of arsenic (As(III)) in wastewater. The structure and properties of the mineral-based composite were characterized by X-ray diffraction (XRD), infrared spectroscopy (IR), scanning electron microscopy (SEM), and photocurrent measurements. The photocatalytic activity of 2D-2D B/g-C3N4 for As(III) removal was further investigated under visible light . The results reveal that the As(III) oxidation rate by 2D-2D B/g-C3N4 composite was three times higher than that by pure g-C3N4, owing to the enlarged specific surface area and the suppressed electron–hole recombination by the incorporated bentonite. Moreover, the composite exhibited a high photocatalytic oxidation efficiency in a wide pH adaptability from 3 to 8.5. Through electron spin resonance (ESR) technique and radical quenching experiments, the photocatalytic mechanism of As(III) oxidation was proposed, where superoxide radicals played a critical role in the photo-oxidation of As(III) in both acid and basic conditions. This work paved a new way to design the mineral-based photocatalyst for treatment of pollutants in a wide pH range.
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Advanced Healthcare Materials
·
2021
·Vol. 10
·期 18
·2100518
·
IF 9.933
Xingyi Xu,Rongyuan Zhang,Xianfeng Yang,Yao Lu,Zhongmin Yang,Mingying Peng,Zhijun Ma,Ju Jiao,Lihua Li
Triple-negative breast cancer (TNBC) exhibits aggressive behavior and high levels of metastasis owing to its complex heterogeneous structure and lack of specific receptors. Here, tumor cell membrane (CM)-coated bismuth/manganese oxide nanoparticles (NPs) with high indocyanine green (ICG) payload up to 50.6 wt% (mBMNI NPs) for targeted TNBC therapy are constructed. The extra-high drug load Bi@Bi 2 O 3 @MnO x NPs (honey-comb like structure) are formed by Kirkendall effect and electrostatic attraction. After modified with CM, they can home into tumor sites precisely, where they respond to internal overexpressed glutathione (GSH), releasing Mn 2+ for chemodynamic therapy (CDT) with GSH depletion, while H 2 O 2 degrades into O 2 enabling relief of tumor hypoxia. In response to external near-infrared irradiation, mBMNI NPs intelligently generate vigorous heat and single oxygen ( 1 O 2 ) for photothermal therapy (PTT) and photodynamic therapy (PDT) owing to high load. Importantly, O 2 production and GSH consumption during the internal response reinforce external PDT, while the heat generated through PTT during the external response promotes internal CDT. The honeycomb-like structure with high ICG load and mutual reinforcement between internal and external response results in excellent therapeutic effects against TNBC.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jianhua Sha,Lulu Li,Zexiu An,Maoxia He,Haiyan Yu,Yao Wang,Baoyu Gao,Shiping Xu
Coexistence of heavy metals usually shows great impact on antibiotics removal. In this study, we firstly reported that Cu 2+ shows diametrically opposite effect on adsorption-photodegradation of sulfamerazine (SMZ) and ciprofloxacin (CIP) in g-C 3 N 4 /visible light system. Cu 2+ can greatly promote CIP adsorption, but showed negligible impact on its degradation, whereas, no obvious influence on SMZ adsorption was recorded, but strong inhibition to its photodegradation was observed. With help of several spectroscopy approaches and DFT calculation, functional mechanism of Cu 2+ on the adsorption-photodegradation of SMZ and CIP was proposed. The main reasons for their different behaviors were found to be their distinct surface charge, spatial structure, electron distribution and complexation with Cu 2+ . Among them, effect of complexation played the most important role in depressing the reactivity of antibiotics during photodegradation . Aiming at retarding this inhibition, an effective approach with idea of complexation replacement was proposed. This study indicated that interactions between antibiotics and heavy metals are very specific, and an appropriate treatment scheme should be given based on systematic study targeting at the specific pollution system.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Renji Zheng,Jing Li,Runliang Zhu,Ranhao Wang,Xuezhen Feng,Zhijie Chen,Wenfei Wei,Dazhong Yang,Hong Chen
Wastewater with complex compositions of both heavy metals and organic pollutants is of critical environmental and socioeconomic threat worldwide, which urgently requires feasible remediation technologies to target this challenge. In this study, natural chalcopyrite (CuFeS 2 , NCP), the most abundant copper-based mineral in the Earth's crust , has been discovered to be a heterogeneous catalyst that can activate peroxydisulfate (PDS) for the simultaneous degradation of organic pollutant Rhodamine B (RhB) and reduction of hexavalent chromium (Cr(VI)). Batch experimental results indicate that both RhB and Cr(VI) could be simultaneously removed under a near-neutral condition in NCP/PDS combined system. The radicals SO 4 •− and • OH generated from PDS activation are the main oxidative species detected by electron paramagnetic resonance (EPR) spectroscopy. SO 4 •− acted as a predominant role in RhB degradation, while Cr(VI) reduction is mainly attributed to the oxidization of S 2− and S 2 2− species on NCP surface, as well as the photoreduction performance of NCP, which could be enhanced by the intermediates generated from RhB degradation. Density functional theory (DFT) calculation results disclose that Fe is the critical catalytic site for PDS activation. This work demonstrates a user-friendly strategy for remediation of complex wastewater containing both heavy metal and organic pollutants by combining photoreduction and advanced oxidation processes (AOPs) with natural minerals. It paves a way for wastewater treatment by utilizing low-cost natural abundant minerals as catalysts.
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Journal of Cleaner Production
·
2021
·
IF 9.297
Yi Chen,Mengjia Ran,Ziyan Zhou,Xinyi Han,Honglin Zhu,Jinchuan Gu
Titanium dioxide (TiO 2 ) is an effective photocatalyst for organic removal. However, its efficacy is hampered by the recombination of photogenerated electrons and holes. This paper presented an eco-friendly, synthetic lanthanum (La)/TiO 2 supported on lithium silicon powder (L) to significantly improve photocatalysis . The results showed that 74.4% dimethyl phthalate (DMP) removal was achieved in the ultraviolet (UV)-La-TiO 2 /L (LTL1) system, which was considerably higher than UV-TiO 2 /L (TL) (60.1%) and UV-L (18.3%). The enhanced LTL1 photocatalysis was based on the synergic effect between TiO 2 and La with L matrix. The photocatalysis efficiency was further improved by hydrogen peroxide (H 2 O 2 ), while the DMP removal rate reached 100% in the UV-LTL1-H 2 O 2 system. The DMP activation mechanisms and degradation pathways in the UV-LTL1-H 2 O 2 system were carefully examined, revealing that increased hydroxyl free radical (OH • ) and superoxide ion radicals (O 2 − • ) were pivotal to the higher degradation rate . Overall, the findings suggested that LTL1 showed considerable application promise for the low-cost and eco-friendly organic removal from water.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Mingjie Huang,Sisi Peng,Wei Xiang,Chen Wang,Xiaohui Wu,Juan Mao,Tao Zhou
This study has revealed how the strong metal-support interaction (SMSI) between carbon nanotubes (CNTs) and Mn 0.65 Fe 2.35 O 4 (MnFeO) in boosting peroxymonosulfate (PMS) activation for rapid sulfamethoxazole (SMX) degradation. As synergized by CNTs, the PMS-activation efficiency of MnFeO could be enhanced by>24 times, but with the similar PMS-activation mechanism. It was explored that the SMSI-induced abundant surface hydroxyl groups, in cooperation with the highly hydrophobic CNTs, favored the rapid in situ interfacial degradation of SMX. This feature also endowed the MnFeO-CNTs catalyst resistance to high salinity waters containing inorganic anions (e.g., Cl - and NO 3 – ) of weak complexing abilities. Moreover, the SMSI allowed the greatly accelerated redox cycle rate of Mn species by electron-rich CNTs, resulting in efficient PMS activation. Furthermore, the application feasibility of the MnFeO-CNTs/PMS system was demonstrated for a SMX-spiked real reverse osmosis (RO) concentrate. It was found that higher concentration of PMS could realize the complete removal of SMX, despite the existence of electron-rich tyrosine-like substances would compete with the SMX degradation in the MnFeO-CNTs/PMS system. This study demonstrated that the SMSI could boost the PMS activation , and could serve as an effective material strategy for in situ interfacial organics degradation in the high salinity wastewater.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Daniel T. Oyekunle,Dan Li,Li Zheng,Fang Luo,Songlin Wang,Zhuqi Chen
Peroxymonosulfate (PMS) has been activated for the generation of reactive oxygen species by nitrogen-doped carbonaceous material . However, the influence of phosphate on the degradation performance has not been reported. In this study, phosphate ions accelerate PMS decomposition and degradation of target organic compounds such as carbamazepine , atrazine , sulfamethoxazole , and benzoic acid . It was revealed that the physical mixture of phosphate with Co and N doped graphitic carbon (GcN/Co) demonstrates the occurrence of P C, P N, and P O – C bonds. Essentially, the graphitic N or graphitic N P increased in the presence of phosphate. This was correlated with the lower electrical transfer resistance, improved electrical conductivity , and higher electron morbidity confirmed by different electrochemical tests. Moreover, due to the strong buffering capacity of phosphate at neutral pH, bicarbonate was used to confirm the negligible influence of pH. The presence of phosphate helps to recover the scavenging effect of Cl – but has no effect on the presence of HCO 3 – and CO 3 2– . Nevertheless, GcN/Co demonstrates good reusability for three reaction cycles, however, in order to maintain a high catalytic performance phosphate needs to be replenished after each cycle.
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Nano Research
·
2021
·Vol. 15
·期 3
·1973-1982
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IF 8.897
Tan Xianjun,Ding Wenhui,Jiang Zhenying,Sun Linxiao,Huang Yuxiong
To better understand the mechanisms of hydrogen peroxide (H 2 O 2 )’s decomposition and reactive oxygen species (ROS)’s formation on the catalyst’s surface is always a critical issue for the environmental application of Fenton/Fenton-like reaction. We here report a new approach to activate H 2 O 2 in a co-catalytic Fenton system with oxygen incorporated MoS 2 , namely MoS 2− x O x nanosheets. The MoS 2− x O x nanosheets assisted co-catalytic Fenton system exhibited superior degradation activity of emerging antibiotic contaminants (e.g., sulfamethoxazole). Combining density functional theory (DFT) calculation and experimental investigation, we demonstrated that oxygen incorporation could improve the intrinsic conductivity of MoS 2− x O x nanosheets and accelerate surface/interfacial charge transfer, which further leads to the efficacious activation of H 2 O 2 . Moreover, by tuning the oxygen proportion in MoS 2− x O x nanosheets, we are able to modulate the generation of ROS and further direct the oriented-conversion of H 2 O 2 to surface-bounded superoxide radical (·O 2 surface − ). It sheds light on the generation and transformation of ROS in the engineered system (e.g., Fenton, Fenton-like reaction) for efficient degradation of persistent pollutants.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Jinyan Cao,Yue Jing,Zhongxing Du,Wei Chu,Jianjun Li,Wanglai Cen
A novel n-n type WC/BiOCl binary photocatalyst was synthesized, and applied to sulfamethoxazole (SMX) degradation. The physical and photoelectric properties of the WC/BiOCl were characterized by various experimental and calculational methods. An intimate interfacial contact between WC and BiOCl was identified, which help to reduce the aggregation of BiOCl and more importantly, build an internal electrical field between WC and BiOCl. It is interesting to find that the WC layer(s) can help to reduce the interfacial charge transfer resistance and act as electron transfer and storage sites. Subsequently, the holes are engaged in the oxidation of SMX by WC/BiOCl. Additionally, WC/BiOCl photocatalyst has more reactive sites and absorbs more incident photons compared with pure BiOCl. Quenching and electron spin resonance (ESR) experiments indicate that O 2 ·- is the main active species, holes and OH • are also involved. The degradation pathway of SMX and the enhancing mechanism for the photodegradation through the combination of WC and BiOCl were explored. This work provides a novel binary photocatalyst for SMX degradation.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Biao Zhu,Qianxin Xu,Xiaoyan Bao,Hao Yin,Yumei Qin,Xing-Can Shen
Sunlight-driven photocatalytic CO 2 into useful carbon compounds is an ideal way to mitigate the greenhouse effect. However, this strategy is limited by poor light absorption and rapid photoexcited electron-hole recombination of traditional photocatalysts. Here, a g-C 3 N 4 (CN) foam/LDH heterojunction monolith (NCF) was fabricated by growing NiFe-LDH in situ on the porous CN foam substrate. The composite had good air permeability and light transmittance, which improves light-harvesting, CO 2 capture, and interfaces charge transfer of the NCF. The results show that the NCF catalyst has good CO 2 adsorption performance (1.52 mmol g −1 ) and enhanced CO 2 photoreduction activity (55.1 μmol g -1 h −1 ), which is ∼ 10 times higher than that of pure LDHs powder. Furthermore, the practical applicability of the NCF monolith with different thicknesses is illustrated via the CO 2 photoreduction test for the first time. This work could shed light on the development of dual-functional materials for efficient capture and photoreduction of CO 2 .
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zhiqun Xie,Zhiping Lyu,Jinnan Wang,Aimin Li,Philippe François-Xavier Corvini
Ultrafine-Mn 2 O 3 @N-doped porous carbon hybrids [Mn 2 O 3 @NC] derived from Mn-MOFs was constructed with 1 O 2 and O 2 −• 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 1 O 2 via chain reaction. Notably, the porous structure of N-doped carbon shell could not only facilitate free radical recombination for generation of 1 O 2 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 1 O 2 , Mn 2 O 3 @NC achieved high mineralization of BPA at low-dose peroxymonosulfate (0.033 g/L).
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Shuzhao Pei,Han Shi,Jinna Zhang,Shengli Wang,Nanqi Ren,Shijie You
This study reports fluorine-doped titanium suboxide anode for electrochemical mineralization of hydrophobic micro-contaminant, tetrabromobisphenol A. Fluorinated TiSO anode promoted electro-generated hydroxyl radicals (•OH) with higher selectivity and activity, due to increased O 2 evolution potential and more loosely interaction with hydrophobic electrode surface. For electro-oxidation process, fluorine doping had an insignificant impact on outer-sphere reaction and exerted inhibition on inner-sphere reaction, as indicated by cyclic voltammogram performed on Ru(NH 3 ) 6 3+/2+ , Fe(CN) 6 3−/4− and Fe 3+/2+ redox couple. This facilitated electrochemical conversion of TBBPA and intermediates via more efficient outer-sphere reaction and hydroxylation route. Additionally, generated O 2 micro-bubbles could be stabilized on hydrophobic F-doped TiSO anode, which extended the three-phase boundary available for interfacial enrichment of TBBPA and subsequent mineralization. Under action of these comprehensive factors, 0.5% F-doped TiSO electrochemically reactive membrane could achieve 99.7% mineralization of TBBPA upon energy consumption of 0.52 kWh m −3 at current density of 7.8 ± 0.24 mA cm −2 (3.75 V vs SHE) and flow rate of 1628 LHM based on flow-through electrolysis. The modified anode exhibited superior performances compared with un-modified one with more efficient TBBPA removal, less toxic intermediate accumulation and lower energy consumption. The results may have important implications for electrochemical removal and detoxification of hydrophobic micro-pollutants.
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