CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Bing Wang,RuiQing Zhang,HuiYong Chen,Zhuo Li,EnZhou Liu,HaiXia Ma,Bo Zhou,Hong Hao,LinYu Jiao
Controllable fine-tuning of heterojunction interfaces at the atomic level represents a promising strategy for enhancing semiconductor photocatalytic performance. Herien, we propose a strategy to introduce hydrogen-bonded electron channels at the heterojunction interface to achieve rapid interfacial electron transfer. This S-scheme hydrogen-bonded supramolecular self-assembled H 12 SubPcB-OPhCH 2 COOH/Ag 3 PO 4 semiconductor heterojunction exhibits efficient and stable photocatalytic degradation of a wide range of pharmaceuticals and personal care products. Experimental results and theoretical simulations demonstrate that the interface O-H⋅⋅⋅O hydrogen bond at the heterojunction generates an internal electric field, which provides the driving force for accelerated S-scheme charge transfer and enhanced redox properties. Furthermore, the combination of TDDFT calculations and synchronous illumination XPS has revealed that hydrogen bonding acts as a suction electron pump in the excited state, transferring electrons from Ag 3 PO 4 to SubPc-2. These findings suggest that hydrogen-bonded supramolecular semiconductor can be used to develop high-performance photocatalytic materials for environmental remediation.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Hui Wang,Yuhan Xiong,Yi He,Lingru Kong,Lan Ding,Rui Wu,Xin-Lei Gao,Jie Ding,Nanqi Ren
Covalent organic frameworks (COFs) have attracted great attention in photocatalysis, but the high recombination rate of photo-induced electron − hole pairs limits their photocatalytic performance. We report a synergy strategy based on the donor − acceptor (D-A) effect and Au clusters to enable the effective transfer and separation of photogenerated electrons to rationally fabricate visible light driven photocatalyst (MT-COF-Au) for the degradation of benzotriazole (BTA). MT-COF-Au displayed superior photocatalytic activity. The degradation efficiency of BTA was 93 % within 110 min, which was significantly improved 6.7 times than COF. For BTA degradation, O 2 − played a prominent role based on reactive species trapping experiments. The products of the last stage of the reaction were ketone, imidazole, acetamide, and nitrogen, which were formed via ring opening and isomerization reactions. MT-COF-Au could be reused for at least 5 cycles without significantly deteriorating its catalytic activity. Experiments and theory calculations confirmed the electron transfer mode and photocatalytic mechanism. This work provides new prospects for the design and synthesis of high-efficiency photocatalyst photocatalysts.
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 48
·期 4
·1757-1770
·
IF 3.3
Ling Tao,Jiepu Zhang,Fangke Yu
In this study, in order to achieve efficient activation of persulfate, we added MoS2 as a co-catalyst to the iron, cobalt and nitrogen modified biochar (Fe–Co–N–BC) catalytic system. Analytical methods such as scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD) demonstrated that the MoS2/Co–Fe–N–BC catalytic materials were successfully prepared. In the MoS2/Fe–Co–N–BC/PMS system, 97.5% of PFOA was removed within 180 min with Kobs of 0.074 min−1. Composites with different mass ratios of MoS2 and Co–Fe–N–BC/PMS in the non-homogeneous PMS system both exhibit excellent catalytic efficiency for TOC removal. In particular, MoS2/Fe–Co–N–BC obtained extraordinary catalytic efficiency through synergistic radical (SO4˙−, ˙OH) and non-radical (1O2, FeIV and FeV) processes, which was proved by the quenching experiments and the EPR testing. The analysis of the activation mechanism reveals that the three redox ion pairs Fe2+/Fe3+, Co2+/Co3+ and Mo4+/Mo6+ simultaneously participated in the activation of PMS, realizing multi-path electron transfer. And MoS2 played an excellent co-catalysis role in promoting the cycling of the valence states of the ions. Compared to Fe3+ and Co3+, the low valence states of Fe2+ and Co2+ can activate PMS more rapidly and produce more ˙OH and SO4˙−. However, the recycling efficiency of Fe2+ and Co3+ in the Fe–Co–N–BC system is low, and the presence of MoS2 improves the efficiency of Fe3+ and Co3+ reduction to Fe2+ and Co2+, respectively. The possible degradation pathways of PFOA were proposed. This study provides some references for the design of polymetallic-doped catalysts to degrade difficult-to-degrade organic pollutants.
✓ 已验证
产品关联
DOI
高影响因子
Crystals
·
2023
·Vol. 13
·期 12
·1664
·
IF 2.7
Yulong Chen,Yuan Chi,Xiao Wu,Cong Lin,Tengfei Lin,Min Gao,Chunlin Zhao,Baisheng Sa
The widespread use of pharmaceuticals and personal care products (PPCPs) in many fields has brought convenience to human lives but has also caused unavoidable environmental pollution issues. In particular, the resistance gene problem resulting from accumulating antibiotics that cannot be fully absorbed by biological individuals has been a concern; thus, it is urgent to find efficient technologies to boost the degradation efficiency of antibiotics in the environment. Here, an ε-MnO2catalyst was prepared by a novel droplet-interface-drying method and utilized as a Fenton-like catalyst for efficiently degrading ciprofloxacin (CIP). The ε-MnO2shell was formed preferentially at the gas–liquid interface and then continued to decompose into ε-MnO2with abundant O vacancies in the air-insulated microcavity. The XPS result confirms that this particular preparation method can regulate the content of O vacancies in the material. Compared with ε-MnO2samples obtained by the direct drying method (ε-MnO2-B), the catalytic performance of ε-MnO2prepared by the droplet-interface-drying method (ε-MnO2-P) is significantly improved. By activating peroxymonosulfate (PMS) with the ε-MnO2-P catalyst, the CIP degradation efficiency can reach 84.1%. The detection and analysis of reactive oxygen species (ROS) in the ε-MnO2-P/PMS oxidation system confirms that ·OH, SO4·−and1O2are the main ROS for CIP degradation. This study highlights the creation of miniature hypoxic space to regulate the content of O vacancies in ε-MnO2, providing a new idea for the synthesis of other O-vacancy-rich materials.Keywords:droplet-interface-drying method;Fenton-like oxidation;ε-MnO2;ciprofloxacin;water purification
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Jie Tian,Yumeng Qi,Junyan Wei,Ahmed Rady,Saleh Maodaa,Ahmed A. Allam,Zunyao Wang,Ruijuan Qu
The degradation process of bisphenol S (BPS) in ozone/peroxymonosulfate (O 3 /PMS) system was systematically explored. The results showed that the removal efficiency of BPS by O 3 could be significantly improved with addition of PMS. Compared with ozonation alone, the pseudo-first-order constant ( k obs ) was increased by 2–5 times after adding 400 μM PMS. In O 3 /PMS system, accelerated removal of BPS was observed under neutral and alkaline conditions. The removal efficiency of BPS reached 100% after 40 s of reaction at pH 7.0, with the k obs of 0.098 s −1 . Moreover, Cu 2+ had a catalytic effect on the O 3 /PMS system, because it could catalyze the decomposition of ozone and PMS to produce •OH and SO 4 •- , respectively. Electron paramagnetic resonance illustrated that •OH and SO 4 •- were the reactive species in O 3 /PMS system. Twelve intermediates were identified by mass spectrometry, and the degradation reactions in O 3 /PMS system mainly included hydroxylation, sulfate addition, polymerization and β-scission. Finally, the toxicity of the products was evaluated by the EOCSAR program. Our results introduce an efficient method for BPS removal and would provide some guidance for the development of O 3 -based advanced oxidation technology .
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·
IF 5.8
Bao Siqi,Yu Xiaotong,Li Xiaolin
Antibiotic contamination has a significant negative impact on China, one of the largest producers and consumers of antibiotics worldwide. In this study, a three-dimensional flower-like structure of CoFe-LDHs was used to efficiently degrade tetracycline (TC) in a system triggered by peroxymonosulfate (PMS) and exposed to visible light. After exploring the effects of different metal ratios, catalyst dosage, initial TC concentrations, and pH, the optimal reaction conditions were determined. In comparison to pure CoFe-LDHs, the TC elimination rate was dramatically increased by the addition of the PMS. The strong environmental resistance, excellent stability and reusability, and universal flexibility were shown. The quenching experiments and electron spin resonance detection showed that the creation of reactive oxygen species was facilitated by the synergistic transmission of electrons between the active bimetallic components. Further, photogenerated holes was the dominant oxidizing species, which contributed more to the degradation of TC. The potential degradation pathways and intermediate toxicity of TC were suggested. This work offers a new method dominated by photogenerated holes for efficiently removing TC effluent.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Yanan Dong,Dong Wang,Yingchen Zhu,Qianwen Wang,Guocheng Liu,Qinghua Yan,Yucan Liu,Qinghua Chen,Dong Ma,Guangshan Zhang,Shuaishuai Xin,Yanjun Xin
The self-sufficient heterogeneous photo-Fenton (SH-PF) system was constructed for doxycycline hydrochloride (DOH) degradation with hydroxyapatite (Hap) modified CuFeO 2 (Hap/CuFeO 2 ) composites through H 2 O 2 in-situ production. The modification of Hap could improve the specific surface area, visible-light response, light conversion efficiency, photoelectron lifetime and oxygen vacancies (OVs) of CuFeO 2 , which was conducive to H 2 O 2 production and DOH degradation in SH-PF system. Notably, Hap/CuFeO 2 fabricated with 0.5 g Hap (Hap/CuFeO 2 -0.5) displayed more superior performance for DOH degradation compared to other synthesized catalysts. The Hap/CuFeO 2 -0.5 load and initial solution pH for DOH degradation in SH-PF system were optimized, and the Hap/CuFeO 2 -0.5 had good reusability and stability. The • OH was the main active species for DOH degradation, and the facilitation effect of • O 2 – and photoelectrons on DOH degradation was associated with the H 2 O 2 production in the present work. In addition, the capture of photogenerated holes suppressed the recombination of photogenerated carriers, elevating the production of photoelectrons and thereby enhancing H 2 O 2 production and DOH degradation. The degradation pathways for DOH were proposed and the comprehensive toxicities of DOH were relieved after degradation in SH-PF system.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ying Wu,Chi Song,Xinyan Yu,Xianbao Shen,Lijie Xu,Ying Zhang,Han Gong,Changlei Xia,Lu Gan
In this study, waste polyethylene (PP) obtained from obsoleting water purifier filter was mixed with ferric chloride hexahydrate (FeCl 3 ·6H 2 O) to prepare a series of single crystal phased iron compound incorporated carbon composites (Fe/PP-C). The prepared Fe/PP-Cx catalysts were then utilized to degrade sulfamethoxazole (SMX) in water by activating peroxymonosulfate (PMS). The results showed that with the assistance of pyrolysis temperature regulation, waste PP filter could control the crystalline phase of the iron compound in the prepared Fe/PP-Cx through releasing distinct gaseous atmospheres at respective pyrolysis temperature. When the pyrolysis temperature was set at 600 °C and 900 °C, pure phase ferric oxide (Fe 3 O 4 ) and zero-valent iron (ZVI) incorporated carbon catalysts were obtained, respectively. 0.2 g/L of Fe/PP-Cx could completely degrade 0.02 mM of SMX within 20 min, in which the toxicity of the reaction solution was also effectively reduced. In both Fe/PP-Cx/PMS systems, non-radical mechanisms dominated the SMX degradation, in which singlet oxygen played the dominant role in the Fe/PP-C600/PMS system, whereas electron transfer process was primarily responsible for SMX degradation in the Fe/PP-C900/PMS system. High-valent iron-oxo species was also involved in SMX degradation in the Fe/PP-C900/PMS system. Since Fe/PP-C600 and Fe/PP-C900 respectively activated PMS via heterogeneous and homogeneous routes, Fe/PP-C600 maintained higher longtime use stability. This study aims to present a simple approach to manipulate the nonradical organic pollutant degradation mechanisms in PMS activated system, which also provides a new strategy of utilizing waste polymer.
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Lianyang Huang,Jiahui Zheng,Jiaqi Ke,Jiahong Pan,Lingling Zhuang,Menglu Zhang,Weifang Zhang
Tetracycline's (TC) incomplete self-photolysis by light irradiation generally produces toxic intermediate products, which posing serious harm to the aqueous environment. In order to diminish the environmental risks of TC self-photolysis, an iron(III)-alginate (Fe-SA) hydrogel assisted photocatalytic method was developed and the underlying mechanisms was also analyzed in this work. Under simulated sunlight, the photo-degradation efficiency of TC was 61.1% at pH 7.0 within 2 h. Importantly, four of the seven intermediate products that identified during the self-photolysis of TC were found toxic based on QSAR analysis. In contrast, the removal efficiency of TC could be improved to 87.4% by adding Fe-SA under the same conditions. Moreover, only two relatively weakly toxic intermediate products were detected after exposing to the Fe-SA photocatalytic system, indicating a significant reduction of the potential ecological risks caused by TC self-photolysis. Furthermore, the determination of reactive oxidation species (ROS) demonstrated that the addition of Fe-SA primarily facilitated the degradation of TC and the related toxic intermediate products through assisting the free radical (∙OH and ∙O 2 − ) photocatalytic degradation pathway. Additionally, the photocatalytic application under actual sunlight conditions and the reusability experiments of Fe-SA further confirmed its effectiveness and low cost in removing TC. This study revealed the photodegradation mechanisms of TC from the perspective of the self-photolysis process, and also offering new insights into the removal of TC pollution in the environment.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Linlin Sun,Xiaoshuo Liu,Huiling Ji,Xunlei Ding,Nan Jiang,Jigang Wang
A large number of residual amino groups may be formed in graphitic carbon nitride (g-C 3 N 4 ), leading to the destruction of active sites and increased carrier recombination centers. Herein, we develop a meaningful material (benzo[b]thiophene-3-carboxaldehyde post-grafting three-dimensional agaric-shaped g-C 3 N 4 (3DA-CN): CNBT) that solves the problems above by prolonging the delocalization of π electrons and changing the intrinsic semiconductor properties. CNBT has a special hierarchical structure, excellent visible light absorption capacity and high carrier separation efficiency. The introduction of BTC promotes the activation of O 2 and spontaneously produces more H 2 O 2 . The H 2 O 2 production rate of CNBT-7 is 2249 μM in 2 h, which is 5.95 times higher than that of 3DA-CN (378 μM). The formation rate constant value of CNBT-7 (31.45 μM·min −1 ) increased to 8.71 times higher than that of 3DA-CN (3.61 μM·min −1 ). The H 2 O 2 production mechanism follows two-step single electron reaction path and has been deeply studied by experiments and density functional theory (DFT) calculations. This work provides a meritorious activity strategy to enhance photocatalytic H 2 O 2 production.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Mengyang Lu,Hanmin Zhang,Yu Tian,Wei Yao,Junsheng Wang,Yuezhu Wang
The integration of catalytic oxidation with forward osmosis (FO) holds promising potential to address two crucial challenges encountered by FO: fouling and unsustainable performance, but suitable approaches are still rare. Herein, we have successfully developed a photocatalysis-assisted forward osmosis (PFO) system. In the PFO, a self-made porous carbon nitride doped functional carbon nanotube photocatalytic hydrogel film (PCN@CNTM) was engaged in the FO process in an inventive way by simply sticking to the commercial FO membrane surface, preventing damage to the membrane from the catalyst's direct insertion and delaying the assault from the oxidation groups. PFO allowed organic pollutants to decompose in the feed solution (90%) and on the membrane surface, regulating the water chemical potential and giving the FO membrane antifouling properties. This resulted in sustainable water flux (11.8 LMH) with no significant membrane fouling in PFO, whereas in FO alone there was a significant fouling and flux drop (from 12.73 to 7.23 LMH in 4 h). Moreover, the expensive FO membrane was protected while the hydrogel film can be replaced on demand. The PFO exemplifies the concept of synergistic technology integration, presenting a new perspective on harnessing the strengths of distinct technologies in a mutually beneficial manner.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Jiaming Zhang,Chao Yu,Longqian Xu,Zhenyu Zhao,Deli Wu
Electro-enhanced metal-free boron/peroxymonosulfate (B/PMS) system has demonstrated potential for efficient metal-organic complexes degradation in an eco-friendly way. However, the efficiency and durability of the boron activator are limited by associated passivation effect. Additionally, the lack of suitable methods utilizing in-situ recovery of metal ions liberated from decomplexation causes huge resource waste. In this study, B/PMS coupled with a customized flow electrolysis membrane (FEM) system is proposed to address above challenges with Ni-EDTA used as the model contaminant. Electrolysis is confirmed to remarkably promote the activation performance of boron towards PMS to efficiently generate • OH which dominated Ni-EDTA decomplexation in the anode chamber. It is revealed that the acidification near the anode electrode improves the stability of boron by inhibiting passivation layer growth. Under optimal parameters (10 mM PMS, 0.5 g/L boron, initial pH = 2.3, current density = 68.87 A/m 2 ), 91.8% of Ni-EDTA could be degraded in 40 min, with a k obs of 6.25 × 10 −2 min −1 . As the decomplexation proceeds, nickel ions are recovered in the cathode chamber with little interference from the concentration of co-existing cations. These findings provide a promising and sustainable strategy for simultaneous metal-organic complexes removal and metal resources recovery.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）