Acta Biomaterialia
·
2023
·
IF 9.7
Qiying Lv,Kai Chi,Xiaolei Shi,Miaodeng Liu,Xiaoye Li,Cheng Zhou,Lin Shi,Huiling Fan,Huan Liu,Jia Liu,Yan Zhang,Shuai Wang,Lin Wang,Zheng Wang
Selectively generating active free radical (AFR) in tumor microenvironment (TME) can promote irreversible oxidation of biomolecules and damage tumor cells, resulting in effective tumor inhibition. However, therapeutic efficacy of AFR-based tumor suppression approaches is often limited by insufficient amount of H 2 O 2 or O 2 within TME. To overcome this obstacle, we design a pH/photothermal dual responsive nanosystem ( [email protected] ) for combined photothermal and nanocatalytic therapy in the near-infrared biowindow. Here the Fe single-atom dispersed N, S-doped carbon nanosheets (FeSA) nanozyme is dispersed by phospholipid-polyethylene glycol-amine (DSPE-PEG-NH 2 ), and further loads artesunate (AS) via an amide reaction. Upon 808-nm laser irradiation in TME, the AS is released and further be catalyzed by the FeSA nanozyme to produce cytotoxic C-centered AFRs, and further be accelerated due to the photothermal conversion performance of FeSA (23.35%). The nanocatalytic process of FeSA nanozyme is realized by density functional theory (DFT). The tumor inhibition rates of a CT26 xenograft model is 92% through a photothermal-enhanced nanocatalytic synergistic therapy, and negligible systematic toxicity is observed. This work offers a potential paradigm of multifunctional single atomic catalysts (SACs) for enhancing tumor nanocatalytic therapy. Statement of significance We designed a pH/photothermal dual responsive nanosystem ( [email protected] ) for nanocatalytic therapy: (1) the nanosystem responsively releases AS under 808-nm laser irradiation in TME; (2) FeSA in the nanosystem can act as heme mimetic to convert AS into high cytotoxic C-centered free radicals for nanocatalytic therapy; (3) the photothermal conversion performance of FeSA further enhances the catalytic process to yield abundant AFR. Both in vitro and in vivo results demonstrate that this nanosystem can efficiently inhibit tumor growth through a photothermal-enhanced nanocatalytic synergistic therapy.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 47
·期 7
·3471-3480
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IF 3.925
Qichang Zhang,Yanmin Jia,Jing Chen,Xiaoxing Wang,Luohong Zhang,Zhi Chen,Zheng Wu
In this work, the construction of heterostructures is considered to be an outstanding method to enhance the decomposition ratio in the piezocatalysis process. Piezoelectric BiFeO3/ZnO heterostructure nanomaterials synthesized via a mixing–calcining method exhibit an enhanced piezocatalysis performance through collecting vibration energy to decompose rhodamine B (RhB) dye. After undergoing 180 min vibration, with the different ZnO contents of 0 wt%, 1 wt%, 2 wt%, 3 wt%, 4 wt% and 5 wt%, the BiFeO3/ZnO heterostructures can respectively decompose 73.4%, 87.0%, 96.9%, 92.9%, 67.9% and 55.1% RhB dye. The kinetic rate constant of the RhB dye decomposition is 21.0 × 10−3 min−1 for the BiFeO3/2%ZnO heterostructures, while it is only 7.37 × 10−3 min−1 for the BiFeO3. The reason for the enhanced piezocatalytic dye decomposition ratio may be that the heterostructure effectively separates the positive and negative charges to reduce the recombination of the positive and negative charges. These main medium active species such as hydroxyl radicals (˙OH) in the process of piezocatalysis are confirmed on the basis of the results of both electron spin resonance and active species capture experiments. The BiFeO3/ZnO heterostructures, with a strongly enhanced piezocatalytic dye decomposition performance, offer a promising option to treat wastewater through collecting environmental vibration energy in the future.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Weichen Zeng,Han Zhang,Rui Wu,Luming Liu,Guibai Li,Heng Liang
This study focused on the preparation, characterization, and sulfamethoxazole (SMX) removal performance of the SnO 2 -coated reactive electrochemical membrane (REM). This REM was fabricated by loading SnO 2 on the reduced TiO 2 nanotube arrays (RTNA)-based Ti membrane (TM). Regarding the dopant for SnO 2 , Sb was more effective in boosting the electrocatalytic activity than Bi, and the energy consumption for Sb-SnO 2 -coated REM (TM/RTNA/ATO) was lower than Bi-SnO 2 -coated REM (TM/RTNA/BTO). As for the internal layer, RTNA provided TM/RTNA/ATO with more electroactive surface areas and prolonged the service lifetime. Compared with batch mode, the SMX removal efficiency in flow-through mode was increased up to 8.4-fold. The SMX degradation performances were also affected by fluid velocity, current density, initial SMX concentration, and electrolyte concentration. The synergistic effects of • OH oxidation and direct electron transfer were responsible for the effective removal of SMX. TM/RTNA/ATO was proved to be stable and durable by multi-cycle and accelerated lifetime tests. Its extensive applicability was verified with high removal efficiencies of SMX in the surface water and wastewater effluent. These results demonstrate the promise of TM/RTNA/ATO for water treatment applications.
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2022
·
IF 7.129
Xiaoying Yuan,Guomin Geng,Xu Liu,Zucheng Wang,Zhaoxin Wang,Noor Samad Shah,Jianjun Song,Yingshu Guo,Lingshuai Kong,Shuhua Liu,Wenyu Zhang
Cobalt-based catalysts are expected as one of the most promising peroxymonosulfate (PMS) activators for the removal of organic pollutants from industrial wastewater . However, the easy agglomeration, difficult separation, and secondary pollution of cobalt ions limit their practical application. In this study, a novel, highly efficient, reusable cobalt and nitrogen co-doped monolithic carbon foam (Co-N-CMF) was utilized to activate PMS for ultrafast pollutant degradation . Co-N-CMF (0.2 g/L) showed ultrafast catalytic kinetics and higher total organic carbon (TOC) removal efficiency. Bisphenol A, ciprofloxacin, 2,4-dichlorophenoxyacetic acid, and 2,4-dichlorophenol could be completely degraded after 2, 4, 5, and 5 min, and the TOC removal efficiencies were 77.4 %, 68.9 %, 72.8 %, and 79.8 %, respectively, corresponding to the above pollution. The sulfate radical (SO 4 •- ) was the main reactive oxygen species in Co-N-CMF/PMS based on electron paramagnetic resonance. The ecological structure-activity relationship program analysis via the quantitative structure activity relationship analysis and phytotoxicity assessment revealed that the Co-N-CMF/PMS system demonstrates good ecological safety and ecological compatibility. The Co-N-CMF catalyst has good catalytic activity and facile recycling, which provides a fine method with excellent PMS activation capacity for 2,4-dichlorophenol elimination from simulated industrial wastewater. This study provides new insights into the development of monolithic catalysts for ultrafast wastewater treatment via PMS activation.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 30
·期 13
·35683-35697
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IF 5.19
Tang Xing,Jin Hongyi,Zou Jing,Liu Shupo,Li Fei,Zhou Zhenming
In this study, calcined water treatment plant sludge (C-WTPS) was used as a catalyst for peroxymonosulfate (PMS) activation to simultaneously remove Disperse Blue 56 (DB56) and phosphates. Firstly, the performance of the C-WTPS/PMS system was examined for the degradation of DB56. The results showed that 96.7% of DB56 (400 mg L −1 ) was removed within 60 min in the presence of 4.8 g L −1 PMS and 0.8 g L −1 C-WTPS at pH 3 and 50 °C. Hydroxyl radicals (·OH), sulfate radicals (SO 4· − ), and singlet oxygen ( 1 O 2 ) were generated during the oxidation process, and 1 O 2 was the main active species. The relatively high surface area, proper Fe content, and abundant ketone groups on the catalyst surface were responsible for PMS activation. Furthermore, the possible degradation pathways of DB56 were proposed based on the gas chromatography–mass spectrometry (GC–MS) results. Secondly, the simultaneous removal of DB56 and phosphates by the C-WTPS/PMS system was investigated. Due to the different removal mechanisms, the effects of the initial phosphate concentration and water matrix species on the removal of DB56 and phosphates showed different trends. Reusability tests results showed that C-WTPS had relatively high stability. In addition, the C-WTPS/PMS system exhibited a high decolorization ratio and phosphate removal efficiency in real wastewater tests. This article offers a value-added approach for reusing WTPS as a catalyst for treating organic contaminants and phosphates.
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CHEMOSPHERE
·
2022
·
IF 8.943
Ke Zhang,Quanliu Yang,Yuwen Jin,Peng He,Qiongyao Li,Pan Chen,Jianyu Zhu,Min Gan
The advanced oxidation processes (AOPs) driven by iron-based materials are the highly efficient technology for refractory organic pollutants treatment. In this work, self-modified iron-based catalysts were prepared using secondary mineral as the precursor by one-step pyrolysis process without additional dopants. The prepared catalysts exhibited excellent performance in catalytic degradation of florfenicol (FF), especially C-AJ, which was derived from ammoniojarosite [(NH 4 , H 3 O)Fe 3 (OH) 6 (SO 4 ) 2 ], activated PDS to degrade 93% FF with initial concentration of 50 mg/L. Quenching tests and electron paramagnetic resonance (ESR) studies showed that SO 4 •− , • OH, and • O 2 − were the main reactive species for FF degradation and their contribution degree was SO 4 •− > • OH > •O 2 − . The Fe 0 and the cycle of Fe(II)/Fe(III) both contributed to the PDS activation, and the reduction of Fe(III) to Fe(II) was accelerated by S 2− on the catalyst surface. In addition, Fe 3 O 4 on the C-AJ indirectly catalyzes PDS by promoting electron transfer . The effects of catalyst dosage, PDS concentration, pH, inorganic anions, and real aqueous matrices on FF degradation, TOC analysis, and cycling test were investigated. The results showed that iron-based catalysts have superior environmental durability due to their excellent catalytic properties in the real aqueous matrices with common inorganic anions and pH 3–9 and its steady catalytic capacity with multiple cycles. Overall, this study sheds new light on the rational design of self-modified iron-based composite and develops low-cost technology toward remediation of FF-contaminated wastewater.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Jin-Long Zhu,Shi-Peng Chen,Wei Lin,Hua-Dong Huang,Zhong-Ming Li
It is a daunting task to balance the catalyst stability and exposure of active site of highly efficient immobilizing photocatalyst system for wastewater treatment. In this study, an in-situ mineralization method based on homogeneous system was proposed to directly construct amorphous TiO 2 into cellulose hydrogel network as the crosslinker for efficiently and safely processing wastewater. This unique structure not only endowed TiO 2 /cellulose microsphere (TMS) with an adsorption capacity of 91.7 mg/g on methylene blue, which was approximately 14 times to cellulose microsphere containing commercial TiO 2 nanoparticles, but also made TMS reusable due to its pH sensitive adsorption capacity. More interestingly, TMS exhibited an auto-accelerating process in decomposing Rhodamine B where the degradation intermediate could act as the receptor of photo-regenerated holes to improve photocatalytical activity. In further cyclic test, the degradation rate constant of intermediate-adsorbed TMS was up to 0.02 mg −1 min −1 . Moreover, the intermediate-adsorbed TMS obtained visible light responsive property, including a removal ratio of 86.3 % against tetracycline (c 0 = 20 mg/L) in 120 min. This in-situ cellulose mineralization provides a new sight into the design of hydrogel immobilized catalyst system with high dispersion and active site exposure for efficient and safe water treatment.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jinxiang Zuo,Jimin Shen,Jing Kang,Pengwei Yan,Binyuan Wang,Shuyu Wang,Donglei Fu,Weiqiang Wang,Tianhao She,Shengxin Zhao,Zhonglin Chen
Catalysts used to degrade pollutants are easily limited by surface reaction sites. Herein, we modified the catalyst by doping boron (B) to overcome the above shortcomings. B-doped NiFe 2 O x catalysts with oxygen vacancies (OVs) were synthesized by the sol–gel method to activate peroxymonosulfate (PMS) for 2,4-dichlorophenoxyacetic acid (2,4-D) degradation. 2,4-D is a widely used herbicide in agricultural production. However, it was difficult to be degraded and dangerous to human health. The B-doped NiFe 2 O x (especially 10B-NiFe 2 O x ) exhibited a high catalytic capacity for 2,4-D, aceclofenac (ACF), bisphenol S (BPS) and amidotrizoic acid (DTZ). And the removal rate of 2,4-D in 10B-NiFe 2 O x /PMS system was increased by 26.4 percentage points compared with NiFe 2 O 4 /PMS system. It was verified that B-O-Fe and B-O-Ni were formed. And OVs were formed on the surface of the catalyst after B doping. SO 4 − was confirmed as the major reactive oxygen species (ROS) by quenching experiments. Metal sites and OVs were conducive to the generation of SO 4 − . According to the in situ analysis of the interfacial reaction mechanism, the –OH structure of HSO 5 − and H 2 O could be adsorbed on the OVs sites and combined with the adjacent Lewis acid sites. The cycle of Fe 2+ /Fe 3+ and Ni 2+ /Ni 3+ promoted the interfacial electron transfer of the combined HSO 5 − , and thus generating SO 4 − . The degradation pathways of 2,4-D were proposed through its intermediates and density functional theory (DFT) calculation by the Fukui function. The degradation mechanism included decarboxylation, dechlorination, dehydroxylation, hydroxylation, H-abstraction, bond cleavage and ring opening. This study verified the possibility of highly efficient pollutant degradation by activating PMS with B-doped modified catalyst.
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ACS Nano
·
2023
·
IF 17.1
Chunhua Zhao,Zekun Liu,Chia-Che Chang,Yi-Chia Chen,Qize Zhang,Xiao-Dong Zhang,Chrysafis Andreou,Jiadong Pang,Ze-Xian Liu,Di-Yan Wang,Moritz F. Kircher,Jiang Yang
Triple-negative breast cancer (TNBC) is considered more aggressive with a poorer prognosis than other breast cancer subtypes. Through systemic bioinformatic analyses, we established the ferroptosis potential index (FPI) based on the expression profile of ferroptosis regulatory genes and found that TNBC has a higher FPI than non-TNBC in human BC cell lines and tumor tissues. To exploit this finding for potential patient stratification, we developed biologically amenable phototheranostic iron pyrite FeS2 nanocrystals (NCs) that efficiently harness near-infrared (NIR) light, as in photovoltaics, for multispectral optoacoustic tomography (MSOT) and photothermal ablation with a high photothermal conversion efficiency (PCE) of 63.1%. Upon NIR irradiation that thermodynamically enhances Fenton reactions, dual death pathways of apoptosis and ferroptosis are simultaneously triggered in TNBC cells, comprehensively limiting primary and metastatic TNBC by regulating p53, FoxO, and HIF-1 signaling pathways and attenuating a series of metabolic processes, including glutathione and amino acids. As a unitary phototheranostic agent with a safe toxicological profile, the nanocrystal represents an effective way to circumvent the lack of therapeutic targets and the propensity of multisite metastatic progression in TNBC in a streamlined workflow of cancer management with an integrated image-guided intervention.
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 8
·4013-4019
·
IF 11.9
Jian-Hui Zheng,Ming-Yu Qi,Zi-Rong Tang,Yi-Jun Xu
Semiconductor-based artificial photoredox-catalyzed organic synthesis offers a promising and green opportunity to harness solar energy for green organic chemistry. However, the precise manipulation of product selectivity over semiconductor-based photocatalysts for selective organic synthesis remains challenging. In this work, we report the rational preparation and application of two kinds of cocatalyst, (RuS2 or Cu2S)-decorated monolayer ZnIn2S4, for the selective dehydrocoupling of aromatic amines into tunable CN coupled imines or C–N coupled secondary amines, respectively, under visible light irradiation. The presence of the RuS2 or Cu2S cocatalyst not only facilitates the charge carrier separation and migration owing to the well-matched energy band structure, but also maneuvers the interfacial charge transfer routes for the selectivity switching between CN and C–N product formation. This work would inspire the rational design of ingenious semiconductor-based composites toward selective modulation in heterogeneous photocatalytic organic synthesis.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Fangmin Wu,Jun Nan,Tianzuo Wang,Zhencheng Ge,Bohan Liu,Meng Chen,Xuesong Ye
The activity and selectivity of the cathode towards electrosynthesis of H 2 O 2 are critical for electro-Fenton process. Herein, nickel-foam modified with N, O co-doped graphite nanosheets (NO-GNSs/Ni-F) was developed as a cathode for highly efficient and selective electrosynthesis of H 2 O 2 . Expectedly, the accumulation of H 2 O 2 at pH= 3 reached 494.2 mg L −1 h −1 , with the selectivity toward H 2 O 2 generation reaching 93.0%. The synergistic effect of different oxygen-containing functional groups and N species on the performance and selectivity of H 2 O 2 electrosynthesis was investigated by density functional theory calculations, and the combination of epoxy and graphitic N (EP + N) was identified as the most favorable configuration with the lowest theoretical overpotential for H 2 O 2 generation. Moreover, NO-GNSs/Ni-F was applied in the electro-Fenton process for p-nitrophenol degradation, resulting in 100% removal within 15 min with the kinetic rate constant of 0.446 min −1 and 97.6% mineralization within 6 h. The efficient removal was mainly attributed to the generation of bulk ·OH. Furthermore, NO-GNSs/Ni-F exhibited excellent stability. This work provides a workable option for the enhancement of H 2 O 2 accumulation and the efficient degradation of pollutants in electro-Fenton system.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Zhuoyue Liu,Ke Wang,Danyang Li,Zhenxin Wang,Shengjiong Yang,Heliang Pang,Gen Wang,Dahu Ding,Delu Miao
Mesoporous carbon materials are promising catalysts for peroxydisulfate (PDS) activation for degrading aqueous organic pollutants but limited by the intrinsic inertness. Herein, co-doping of iron and nitrogen into the mesoporous carbon framework was performed via thermal conversion of metal-polyphenol coordination polymers (Fe-TA) to synthesize Fe/N co-doped mesoporous carbon for efficient PDS activation. Owing to the large surface area, high graphitization degree and defective configurations, the Fe/N co-doped mesoporous carbon (Fe/N-MCs) exhibited superior catalytic performance toward the degradation of organic pollutants . Electron paramagnetic resonance tests, chemical quenching experiments, electrochemical analysis and spectra measurements revealed that the degradation of organic pollutants over the Fe/N-MCs followed a nonradical oxidation pathway based on electron transfer process. Graphite nitrogen and hydroxyl (C-OH) groups on the defective edges of Fe/N-MCs were proved to be possible active sites for PDS activation. PDS catalyzed by the Fe/N-MCs exhibited strong anti-interference capability to surrounding inorganic ions (such as Cl – , CO 3 2– , NO 3 – and SO 4 2– ) and natural organic matters, making it a promising candidate for the degradation of organic pollutants. This work provides a new prospect for developing highly active mesoporous carbon materials via heteroatom doping for PDS activation for wastewater decontamination .
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危险品化学品经营许可证（带存储）