Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Adeel Ahmed,Muhammad Usman,Zhijian Ji,Muhammad Rafiq,Raza Ullah,Bing Yu,Youqing Shen,Hailin Cong
In this work, an environmentally friendly reduced graphene oxidized supported cobalt ferrite (CFO/rGO) catalyst was constructed using a hydrothermal technique to heterogeneously activate peroxymonosulfate (PMS) and utilized for the degradation of sulfamethoxazole (SMX) antibiotic in aqueous solution. The results exhibited that the complete degradation of SMX was achieved in 25 min under optimal conditions ([SMX] = 8.0 mg/L, [CFO/rGO-30%] = 0.5 g/L, [PMS] = 5.0 mM, pH = 7.0) in the presence of CFO/rGO-30%/PMS with a rate constant of 0.3076 min ˗1 , which was roughly 6.08 times higher compared to the CoFe 2 O 4 /PMS system (0.0506 min ˗1 ). The enhanced degradation of SMX in the CFO/rGO-30%/PMS system might be attributed to the large surface area of the CFO/rGO-30% (98.11 m 2 /g) catalyst compared to the pristine CoFe 2 O 4 (24.31 m 2 /g), which increased the availability of active sites for PMS activation . Furthermore, the influence of pivotal reaction parameters and interfering anions on SMX mineralization was also scrutinized. The formation of free radicals (SO 4 •− , • OH, and 1 O 2 ) was established through quenching experiments and electron paramagnetic resonance analysis. The degradation mechanism of SMX was speculated based on the identification of degradation intermediates and X-ray photoelectron spectroscopy spectral analysis. Mechanistic investigations suggested that the transition of Co 2+ /Co 3+ and Fe 3+ /Fe 2+ pairs on the catalyst surface was responsible for the PMS activation, and the SMX degradation was accomplished through radical and non-radical pathways. Furthermore, CFO/rGO-30% exhibited high stability after four consecutive cycles and maintained catalytic activity . Finally, the developed CFO/rGO-30% catalyst exhibited promising potential for the purification of SMX polluted water.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Linlin Sun,Xiaoshuo Liu,Yibing Feng,Xunlei Ding,Jigang Wang,Nan Jiang,Shanjiang Wang
A special two-layer coordination configuration anchored single-atom La (SALa) catalyst is synthesized to realize the effective separation of electrons in space and efficient active sites for the activation of O 2 to produce more active species. The special SALa microenvironment is obtained by a novel and facile reduction method that avoids the formation of rare earth oxides and the concentration of loaded SALa (10.34 wt%) exceeds that in most previous studies. The photodegradation test results show that antibiotics are almost completely removed within 30 min by SALa/CN. The first-order kinetic constant of SALa/CN (0.10661 min −1 ) is approximately 9.81 times higher than that of 3DA-CN (0.01087 min −1 ). SALa can be considered as a bridge to transfer electrons and •O 2 − , 1 O 2 and h + are the main active species to degrade tetracycline into some pollution-free small molecules. This work provides an efficient rare earth single-atom catalyst activity strategy possessing certain potential in practical applications.
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ACS Catalysis
·
2023
·
IF 12.9
Heng Shi,Yi He,Yubin Li,Pingya Luo
Fenton-like catalysis based on peroxymonosulfate (PMS) activation has shown great potential in the treatment of organic wastewater. Heterogeneous Fenton-like catalysts containing transition metal active sites are highly efficient for PMS activation. However, the reduction of oxidized metal active sites was usually not prompt due to the sluggish reaction kinetics, which caused the insufficient redox cycle of the metal active sites and further hampered the catalysis efficiency. Recent studies have shown that the synergy effect between photocatalysis and PMS activation may address the above obstacle and boost overall efficiency. However, a deeper understanding of this synergy effect is still missing, making it difficult to be rationally controlled; thus, a poor synergy effect is frequently reported. Herein, a Co/Fe bimetal-doped graphitic carbon nitride (g-C3N4) was designed representatively through systematical characterization and theoretical calculation, the synergy effect was revealed to be profoundly determined by the competitive role of a hole in the system and the adsorbed metastable PMS* on the catalyst surface, and furthermore, the synergy effect can be rationally manipulated; when the Co/Fe doping ratio is 2.5:2.5, the as-prepared g-C3N4 with a moderate valence band position can endow the catalyst with an optimized photo-Fenton-like synergistic effect and the highest catalytic degradation performance. This work sheds light on the rational design of highly efficient photo-Fenton-like catalysts.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Yunning Chen,Zhengkai Wu,Renquan Guan,Xueying Cheng,Qingkun Shang,Yingnan Sun
Improving the efficiency of photogenerated charge separation and transport is the primary goal of designing and constructing efficient composite photocatalysts. The matching of energy bands and the formation of chemical bond between the two components are very conducive to the separation and transmission of photogenerated charges. Herein, three perylene diimide derivatives (PDIs) are synthesized by introducing sulfonic acid group (PDI-SA) and benzenesulfonic acid (PDI-BSA) respectively into the amide bond and further chlorine bay-substituting (Cl-PDI-BSA). The good water solubility of Cl-PDI-BSA ensures its forms a stable chemical bond with TiO 2 through the sulfonic acid group in the single molecular state, coupled with the matching of energy band structure, TiO 2 @Cl-PDI-BSA exhibited excellent performance upon visible light photocatalytic degradation to phenol and trenbolone acetate (TBA). It can remove 100% of phenol in 15 min and 100% trenbolone acetate (TBA) in 30 min, which is 14.3 times that of TiO 2 . Combining to DFT calculation, Kelvin probe force microscope and EPR analysis prove that bay chlorine substitution has a greater impact on the energy band structure and electron cloud distribution of PDIs than N-sulfonation, thereby seriously affecting the transport of photogenerated carriers with TiO 2 .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Shanshan Song,Miao Yang,Fei He,Xiao Zhang,Yijun Gao,Baichao An,He Ding,Shili Gai,Piaoping Yang
Nanozyme-based synergistic catalytic therapies for tumors have attracted extensive research attention. However, the unsatisfactory efficiency and negative impact of the tumor microenvironment (TME) hinder its clinical applications. In this study, we provide an easy method to prepare transition metals loaded onto pyrrolic nitrogen-rich g-C 3 N 4 (PN-g-C 3 N 4 ) for forming metal-N4 sites. This N-rich material effectively transfers electrons from g-C 3 N 4 to metal-N4 sites, promotes the oxidation–reduction reaction of metals with different valence states, and improves material reusability. Under TME conditions, copper ions loaded onto PN-g-C 3 N 4 (Cu-PN-g-C 3 N 4 , CPC) can produce ·OH through a Fenton-like reaction for tumor inhibition. This Fenton-like reaction and tumor cell inhibition can be improved further by a photodynamic effect caused by light irradiation. We introduced upconversion nanoparticles (UCNPs) into CPC to obtain nano-enzymes (UCNPs@Cu-PN-g-C 3 N 4 , UCPC) for effectively penetrating the tissue, which emits light corresponding to the UV absorption region of CPC when excited with 980 nm near-infrared (NIR) light. The nanoplatform can reduce H 2 O 2 concentration upon exposure to NIR light; this induces an increase in dissolved oxygen content and produces a higher supply of reactive oxygen species (ROS) for destroying tumor cells. Owing to the narrow bandgap (1.92 eV) of UCPC under 980 light irradiation, even under the condition of hypoxia, the excited electrons in the conduction band can reduce insoluble O 2 through a single electron transfer process, thus effectively generating O 2 •– . Nanoenzyme materials with catalase properties produce three types of ROS (·OH, O 2 •– and 1 O 2 ) when realizing chemodynamic and photodynamic therapies. An excellent therapeutic effect was established by killing cells in vitro and the tumor-inhibiting effect in vivo , proving that the prepared nanoenzymes have an effective therapeutic effect and that the endogenous synergistic treatment of multiple treatment technologies can be realized.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2023
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IF 11.4
Yishuai Pan,Xiaoshan Zheng,Guoqiang Zhao,Zepeng Rao,Wanchao Yu,Baoliang Chen,Chiheng Chu
The hydroxyl radical (•OH) is a potent oxidant and key reactive species in mediating element cycles and pollutant dynamics in the natural environment. The natural source of •OH is historically linked to photochemical processes (e.g., photoactivation of natural organic matter or iron minerals) or redox chemical processes (e.g., reaction of microbe-excreted or reduced iron/natural organic matter/sulfide-released electrons with O2 in soils and sediments). This study revealed a ubiquitous source of •OH production via water vapor condensation on iron mineral surfaces. Distinct •OH productions (15–478 nM via water vapor condensation) were observed on all investigated iron minerals of abundant natural occurrence (i.e., goethite, hematite, and magnetite). The spontaneous •OH productions were triggered by contact electrification and Fenton-like activation of hydrogen peroxide (H2O2) at the water–iron mineral interface. Those •OH drove efficient transformation of organic pollutants associated on iron mineral surfaces. After 240 cycles of water vapor condensation and evaporation, bisphenol A and carbamazepine degraded by 25%–100% and 16%–51%, respectively, forming •OH-mediated arene/alkene hydroxylation products. Our findings largely broaden the natural source of •OH. Given the ubiquitous existence of iron minerals on Earth’s surface, those newly discovered •OH could play a role in the transformation of pollutants and organic carbon associated with iron mineral surfaces.
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Environmental Science-Nano
·
2023
·Vol. 10
·期 8
·2066-2076
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IF 7.3
Jiahui Zhou,Xuesong Li,Qiuying Yi,Zhiwei Wang
Heterogeneous Fenton-like processes based on Fe-based catalysts are effective technology to degrade emerging organic pollutants in water and wastewater such as tetracycline (TC). However, the kinetically limited redox cycling between Fe2+ and Fe3+ is still a persistent challenge for their widespread application. To address this issue, we designed a novel Fe-based catalyst by coating reduced iron powder (RIP) with ferroferric oxide nanoparticles (FONP@RIP) using a simple chemical co-precipitation method. The reduced iron could rapidly reduce Fe(III) to Fe(II) and accelerate the cycle of Fe(II)/Fe(III) in the heterogeneous Fenton-like system. Benefiting from the accelerated cycle of Fe(II)/Fe(III), TC could be efficiently degraded in the FONP@RIP/H2O2 system over a wide pH range of 3–6, with a removal efficiency of 94.5% within 60 min (TC0 = 150 ppm). The predominant reactive oxygen species were identified as ˙OH and HO2˙. Based on the identified intermediates, the possible pathway of TC degradation was deduced and the toxicity of pollutants could also be significantly reduced during the degradation process. Moreover, FONP@RIP exhibited stable catalytic performance during multiple cyclic tests with only a marginal loss of catalytic components. This study presents a new catalyst design strategy for heterogeneous Fenton-like processes, which provides a promising way for the degradation of residual antibiotics in water and wastewater.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Yu-Ling Yang,Gang Wang,Ping Zhu,Lei Tang,Zhi-Xiang Zeng,Li-Jing Zhu
Membrane separation technology has been widely employed in wastewater separation, although, it is restricted by terrible membrane fouling. The acceptable “single defense” is insufficient to generate a desirable antifouling surface against various organic foulants in complex wastewater. Therefore, this work designs and constructs a porous surface with “multi-defense” by integrating hydrophilic, underwater superoleophobic, and anti-bacterial nano Fe-based Fenton catalysts of β -FeOOH nanorods and CuFeO 2 nanoparticles on the polyvinylidene difluoride membrane via metal-ion-induced deposition process. The obtained composite membrane (M FeOOH/CF ) has ultra-stable underwater superoleophobicity and ultra-low oil adhesion, which prevent oils from adhering to the membrane and benefit to separate various surfactant-stabilized oil-in-water emulsions with high water flux and separation efficiency of 99%. M FeOOH/CF also exhibits nearly 100% bactericidal activity against Escherichia coli. Moreover, the various foulants (such as bovine serum albumin, methylene blue, and crude oil) adhered to the membrane after filtration can be successfully degraded by M FeOOH/CF under the solar-driven Fenton process, leading to ultrahigh flux recovery ratio ( FRRV ) of 98.2 ± 0.3% and a low irreversible fouling ratio ( RirV ) of 2.0 ± 0.1%. The apparent degradation rate constant ( k ) of M FeOOH/CF is 2.5 times the β -FeOOH coated membrane (M FeOOH ) because the introduction of CuFeO 2 nanoparticles provides more reactive sites and lowers the Fe 3+ /Fe 2+ redox potential. This study is working to bring about a highly efficient “multi-defense” on the porous membrane, which will realize membrane regeneration and boost wastewater purification.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Qing Xin,Siqi Liu,Shixu Lu,Zhenyu Chen,Pengzhan Han,Shuaishuai Xin,Qianwen Wang,Guocheng Liu,Chengzhi Zhou,Yanjun Xin,Qinghua Yan
In this study, a fast and efficient Cu 2 Fe 0.5 Al 0.5 -LDH/PMS water purification system was constructed to degrade sulfamethoxazole (SMX). The optimized Cu 2 Fe 0.5 Al 0.5 -LDH/PMS reaction system degraded 50% SMX for only 0.5 min, and 98.25% SMX for 10 min. The advanced characterization techniques proved that the abundant hydroxyl groups of Cu 2 Fe 0.5 Al 0.5 -LDH can form ≡M−(O)OSO 3 − complexes with PMS, resulting in reactive oxygen species (ROS) and promoting SMX degradation. Moreover, the electron transfer between the active bimetallic components played a synergistic role in the generation of ROS species. Compared with the electron transfer degradation mechanism, ROS mechanism contributed more to SMX degradation, in which surface-bound SO 4 − was the dominated active species. The possible degradation pathway and intermediate toxicity of SMX were proposed. This work provided a strategy to fully explore the catalytic degradation mechanism of heterogeneous catalysts in wastewater purification.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Kai Sun,Jiaying Yu,Jinzhong Hu,Wanxiang Yang,Xianfeng Chu,Lucheng Chen,Xiongwei Deng,Baiwang Sun,Zhifei Wang
Ferroptosis is an emerging antitumor treatment modality with the superiority for evading apoptotic cell death pathway. However, how to elevate catalytic efficacy of Fe 2+ -mediated Fenton reaction and efficiently elicit ferroptosis remain enormously challenging. Herein, inspired by hyperthermia-enhanced Fenton reaction kinetics, we firstly designed iron-polyphenol-aspirin-coordinated nanochelates for photothermal-enhanced ferroptosis antitumor immunotherapy. Specifically, we modulated optimal mass feeding ratio of gallic acid (GA), aspirin (ASA), Fe (II) and polyvinylpyrrolidone (PVP) to construct novel nanofibrous GA-ASA-Fe (II) metalchelates named GAFs. The variations in size and structure allowed the nanomedicines to avoid the risk of premature renal clearance in vivo, compared with the reported ultrasmall GA-Fe (II) nanocomplexes (GFs). Under NIR laser irradiation, GAFs could constantly amplify toxic hydroxyl radicals ( OH) generation and deplete excessive GSH to induce more accumulation of lethal lipid peroxidation (LPO), thereby triggering ferroptosis pathway in vitro and in vivo. Besides, the introduction of ASA could inhibit cyclooxygenase-2 (COX-2) and prostaglandin E 2 (PGE 2 ), in combination with photothermal-enhanced ferroptosis tumor therapy to induce immunogenic cell death (ICD), promote maturation of dendritic cells (DCs) and activate cytotoxic T cells for synergistic antitumor immunotherapy. GAFs with laser irradiation exhibited the capacity of inhibition of pulmonary metastasis. This work presented a strategy for incorporating small molecule immunomodulator into the metal-polyphenolic coordination to ameliorate its deficiencies, thereby inspiring a new design concept for tumor treatment.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Yanbin Wang,Zezhou Shi,Haibo Shen,Qiushuang Xing,Yunqing Pi
Efficient and selective removal of organic contaminants using traditional radical-dominated Advanced Oxidation Processes (AOPs) in complex environmental matrices is challenging, especially under high salinity conditions. This study proposes an alternative approach using iron (II) phthalocyanine-supported g-C 3 N 4 composite (FePc/CN) as a peroxymonosulfate (PMS) activator to efficiently remove organic contaminants. The FePc/CN-PMS process was selective towards the elimination of various organic contaminants, and those compounds with lower ionization potential value can be effectively degraded after reaction for 10 min. Results from radical quenching experiments, electron spin resonance (ESR), and PMSO chemical probe indicated that the dominant active species in the FePc/CN-PMS process are high-valent iron-oxo species (Fe IV O 2+ ), rather than the long-recognized SO 4 •− and •OH radical. A total of 22 intermediate products resulting from the degradation of levofloxacin (LVF) were identified by LC-MS. Additionally, two degradation pathways of LVF were proposed, with the piperazine ring of LVF being the primary site of degradation. The 5%FePc/CN-PMS system demonstrates resistance to ubiquitous inorganic anions and dissolved organic matter (DOM) in an aquatic environment, enabling efficient removal of (LVF) even under high salinity conditions. Furthermore, the 5%FePc/CN catalyst exhibits good chemical stability and reusability, making it a viable option for practical water remediation.
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ACS Applied Materials & Interfaces
·
2023
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IF 9.5
Quanhua Deng,Min Han,Haiping Li,Guoan Wang,Wenxuan Hu,Lei Feng,Wanguo Hou
The photoexcited charge separation efficiency of photocatalysts is generally considered as the key factor for enhancement of their photocatalytic activity, and sometimes, their photoabsorption capability and interfacial reaction kinetics play a key part, but the role of interfacial affinity of photocatalysts with substrates was rarely researched systematically. Herein, nitrogen vacancy-modified polymeric carbon nitride porous nanotubes (PCNpts) were simply synthesized, using tartaric acid as a crosslinking and corrosion agent, and exhibit a remarkable increment in surface area, wettability, photoabsorption and charge separation capability, and photocatalytic activity in water splitting to produce H2, but, interestingly, exhibit substrate-dependent variation of photoactivity in contaminant degradation, compared with bulk PCN. More interestingly, the interfacial affinity of PCNpts and PCN with contaminants and H2O, rather than photoabsorption and charge separation capability, is confirmed to dominate their photoactivity.
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