SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Hongyu Wang,Guoqing Wu,Yao Xiao,Zhengfei Zhang,Lei Huang,Meng Li,Henghui You,Zhenxin Chen,Jia Yan,Xianjie Liu,Hongguo Zhang
The increasing amount of heavy metal copper ions (Cu 2+ ) in industrial emissions, poses a serious threat to human health, biological environment, and resource scarcity. Capacitive deionization (CDI) is considered as a green and efficient method for desalination. It is crucial to develop high-performance electrodes for efficient operation of CDI that go beyond conventional carbon and yield considerable environmental benefits. Here, metal organic frameworks (MOFs) derived carbon-loaded cobalt metaphosphate (NC-Co(PO 3 ) 2 ) was prepared by low-temperature gas–solid phosphating for Cu 2+ removal as CDI electrode for the first time. NC-Co(PO 3 ) 2 demonstrated superior electrode structure and function due to the synergistic effects of electric double layer coupling P-O bonds, the binding tendency of metaphosphate groups with Cu 2+ , and interfacial redox reactions induced by the labile valence state of cobalt. The optimal electrosorption capacity of NC-Co(PO 3 ) 2 was 95.41 mg g −1 at 1 V in 50 mL Cu 2+ solution with splendid cyclic regeneration capability. Moreover, NC-Co(PO 3 ) 2 exhibited excellent selectivity and outstanding electrosorption performance in the presence of multiple coexisting ions and this CDI system realized the purification of actual copper-containing wastewater. A series of characterizations further revealed the specific mechanism of Cu 2+ in adsorption–desorption process. Our finding strongly supported NC-Co(PO 3 ) 2 electrode can extend the CDI platform's capability for effectively removing and retrieving Cu 2+ from wastewater.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Kuang Wang,Guan Wang,Long Zhou,Yuan Zeng,Yifeng Zhang,Zhanqiang Fang
The utilization of nano zero-valent iron (nZVI) in polybrominated diphenyl ethers remediation has been studied extensively. However, challenges in balancing cost and reactivity have been encountered. A submicron zero-valent iron coated with FeC 2 O 4 ·2 H 2 O layers (OX-smZVI) was synthesized via a mechanochemical method, aiming to resolve this contradiction. Characterization via SEM, TEM, and XPS confirmed the structure as FeC 2 O 4 ·2 H 2 O coated iron lamellate with a surface area 24-fold higher than ball-milled zero-valent iron (smZVI). XRD highlighted an Fe/C eutectic in OX-smZVI, boosting its electron transfer capacity . Decabromodiphenyl ether degradation by OX-smZVI follows a two-stage process, with initial degradation by FeC 2 O 4 ·2 H 2 O and a subsequent phase dominated by electron transfer . OX-smZVI exhibits a 4.52–34.40 times faster BDE209 removal rate than nZVI and scaled-up OX-smZVI displayed superior reactivity with preparation costs only 1/680 of nZVI. Given its enhanced reactivity and cost-efficiency, OX-smZVI emerges as a promising replacement for nZVI.
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高影响因子
BIORESOURCE TECHNOLOGY
·
2021
·
IF 9.642
Pingbo Wang,Meiying Ye,Yue Cui,Xiong Xiao,Dexun Zou,Rongxin Guo,Yanping Liu
Two-phase high-solid digestion is conducive to the degradation of food waste. In this study, Fe/C was added in high-solid digestion in different acidification and/or methanogenic phase. The experimental results indicated that it significantly increased the cumulative yield of biomethane. When Fe/C was added to the acidification phase only and both the acidification and methanogenic phases, the biomethane yield reached 474.07 ± 7.03 and 475.47 ± 4.68 mL·g VS −1 , respectively, and the biodegradation rate reached 87.30% and 87.58%, respectively, indicating that Fe/C had mainly effect on the performance of acidification phase. In a two-phase anaerobic fermentation system, the activity of dehydrogenases and the concentration of coenzyme F 420 were 2.23–2.95 mg·g −1 ·h −1 and 0.0063–0.0294 mol·g −1 volatile solids, respectively. Additionally, the archaeal communities production pathway of methane from using acetic acid to using hydrogen as the reactant.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Li Gong,Xiaojiang Qiu,Paul G. Tratnyek,Chengshuai Liu,Feng He
FeNX in Fe single-atom catalysts can be the active site for adsorption and activation of reactants. In addition, FeNX species have been shown to facilitate electron transfer between Fe and the carbon supports used in newly developed metal–air batteries. We hypothesized that the combination of FeNX species with granular zero-valent iron (ZVI) might result in catalyzed reductive decontamination of groundwater contaminants such as trichloroethylene (TCE). Here, such materials synthesized by ball milling microscale ZVI with melamine and the resulting N species were mainly in the form of pyridinic, pyrrolic, and graphitic N. This new material (abbreviated as N–C-mZVIbm) dechlorinated TCE at higher rates than bare mZVIbm (about 3.5-fold) due to facilitated electron transfer through (or around) the surface layer of iron oxides by the newly formed Fe–NX(C). N–C-mZVIbm gave higher kTCE (0.4–1.14 day–1) than mZVIbm (0–0.4 day–1) over a wide range of pH values (4–11). Unlike most ZVI systems, kTCE for N–C-mZVIbm increased with increasing pH values. This is because the oxide layer that passivates Fe0 at a high pH is disrupted by Fe–NX(C) formed on N–C-mZVIbm, thereby allowing TCE dechlorination and HER under basic conditions. Serial respike experiments gave no evidence of decreased performance of N–C-mZVIbm, showing that the advantages of this material might remain under field applications.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Mengting Zou,Yumeng Qi,Ruijuan Qu,Gadah Al-Basher,Xiaoxue Pan,Zunyao Wang,Zongli Huo,Feng Zhu
2,4-Dihydroxybenzophenone (BP-1), a typically known derivative of the benzophenone-type UV filter, has been frequently detected in aqueous environments and poses a potential risk to human health and the entire ecosystem. In this study, an effective advanced oxidation technique using zero-valent iron powder (Fe 0 )-activated persulfate (PS) was used for the degradation of BP-1. The effects of several experimental parameters, including Fe 0 dosages, PS dosages, pH, and common natural water constituents, were systematically investigated. The BP-1 degradation efficiency was enhanced by increasing the Fe 0 and PS dosages and decreasing the solution pH. The presence of different concentrations of humic acid (HA) could inhibit BP-1 removal, while the addition of various cations and anions had different effects on the degradation. Moreover, the degradation of BP-1 in five water matrices was also compared, and the removal rates followed the order of ultrapure water > tap water > secondary clarifier effluent > river water > synthetic water. Thirteen oxidation products were identified by liquid chromatography-time-of-flight-mass spectrometry (LC-TOF-MS) analysis, and five possible degradation pathways were proposed. The addition reactions initiated by HO and SO 4 − , as well as single-electron coupling reactions and ring-closing reactions, were further supported by density functional theory (DFT) calculations. Assessment of toxicity of intermediates of the oxidation of BP-1 suggested decreased toxicity from the parent contaminant. The present work illustrates that BP-1 could be efficiently degraded in the Fe 0 /PS system, which may provide new insights into the removal of benzophenones in water and wastewater.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Ningfan Song,Zihan Chen,Jinghua Shi,Dezhi Shi,Li Gu
In the present study, a Pd/Cu bimetallic catalyst supported on a chelating resin (TP207) was prepared in order to selectively reduce nitrate to N 2 with ZVI (zero valent iron) as a reductant. The effects of Pd/Cu mass ratio, temperature, and initial solution pH on the removal of nitrate and TN were then examined. The highest nitrate (63.2%) removal was obtained under neutral conditions at a ratio of Pd/Cu 2:1, in which 57.8% of TN was removed and N 2 accounted for more than 90% of the final products. Additional ammonia (30–40%) were formed when the reaction was conducted at a higher temperature (313 K) compared to when performed at 303 K. The mechanism study for nitrate reduction indicated that this catalyst could broaden the suitable pH range and improve the selectivity of N 2 without the generation of other intermediate compounds or by-products in comparison to ZVI and its combination with a non-supported Pd/Cu catalyst. The slow rate of ZVI corrosion, high Fe(Ⅱ) proportion in corrosion products and high N/H ratio at neutral pH conditions may serve as reasons for the high N 2 selectivity. The chelating resin also played a key role via its load capacity and dispersion ability to Pd/Cu particles in enhancing N 2 selectivity. Accordingly, the proposed method may have great potential application for nitrate reduction to N 2 , which warrants further study.
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CHEMOSPHERE
·
2021
·
IF 7.086
Weitong Tan,Yang Ruan,Zenghui Diao,Gang Song,Minhua Su,Li'an Hou,Diyun Chen,Lingjun Kong,Hongmei Deng
Nano zero-valent iron (nZVI) is widely used for decontamination . The main issues associated with nZVI are agglomeration and oxidation in the long term. In this study, the carbothermal reduction of cotton fiber was conducted for the synthesis of nZVI supported on cotton carbon fiber (nZVI/ CF ) to address the agglomeration and oxidation of nZVI. Synergistic adsorption and peroxymonosulfate (PMS) activation using nZVI/CF for removing levofloxacin (LEV) are reported herein. The nZVI concentration and morphology were conveniently adjusted by soaking cotton fiber in ferric nitrate solutions of various Fe 3+ concentrations. The carbothermal reduction of the cotton fiber at 900 °C contributed to the reduction of Fe 3+ into nZVI. A nZVI/CF-900-0.3 system was obtained through the carbothermal reduction of cotton fiber soaked in 0.3 M ferric nitrate. Favorable adsorption of nZVI/CF-900-0.3 to LEV facilitated LEV degradation under PMS activation. Approximately 93.83% of LEV (C 0 = 20 ppm) was removed within 60 min with 0.2 g/L of the catalyst and 1 mM PMS. It was preferable to use nZVI + CF-900 to activate PMS for degrading LEV, thus confirming the favorable effect of LEV adsorption on further degradation. The nZVI/CF-900-0.3 exhibited excellent long-term stability given that it was able to activate PMS after it was stored for 6 months. ·SO 4 − played an important role in LEV degradation in the presence of PMS.
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Shuang Zhang,Xinxin Ma,Dong Xie,Weijie Guan,Min Yang,Pan Zhao,Ming Gao,Qunhui Wang,Chuanfu Wu
The addition of activated carbon (AC) may improve the efficiency of anaerobic digestion (AD) system to which zero-valent iron (ZVI) has been added. This study investigated the effects of the addition of AC on the AD system with ZVI added. Results showed that the cumulative methane production of 5 g/L ZVI + 5 g/L AC (5ZVI + 5AC) was 2.77–35.0% higher than that of 5 g/L ZVI, 10 g/L ZVI and control. The combined addition shortened the time to reach maximum daily methane yield by 18.2% compared to ZVI groups. Meanwhile, 5ZVI+5AC had the lowest free ammonia concentration (average 461 mg/L) amongst all groups, thus effectively alleviating the ammonia inhibition. Microbial community analysis showed that the combined addition of ZVI and AC enriched hydrogenotrophic methanogens ( Methanoculleus ) and direct interspecies electron transfer related microorganisms ( Syntrophomonas and Methanosaeta ), possibly enhancing electron exchange to accelerate methane production.
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高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Shuxuan Wu,Sheng Deng,Zhifei Ma,Yuhui Liu,Yu Yang,Yonghai Jiang
Zero-valent iron (ZVI), with high reduction capacity and cost effectiveness, has been widely used as an activator for persulfate in remediation of organic pollutants. However, the existence of inherent iron oxide shell blocked the transfer of proton and further reduced its reactivity. In present study, a novel persulfate (PS) activator BZVI@OA was synthesized via ball milling ZVI with oxalic acid dihydrate. Scanning electron microscope , X-ray diffraction spectroscopy, X-ray photoelectron spectroscopy, Fourier transform infrared spectrometry and Time-of-flight secondary ion mass spectroscopy confirmed the original low proton conductive oxidation shell was replaced by a high proton conductive FeC 2 O 4 shell. The generated shell significantly improved persulfate activated capacity, through which degradation rates of various contaminants were enhanced for 1.64 to 2.33 times. Dissolved oxalate was proved to form complexes with iron ions, dramatically reduced the potential difference and relieved the blocked cyclic conversion. Electron paramagnetic resonance and quenching experiments confirmed an inner sphere adsorption of PS on FeC 2 O 4 ·2H 2 O shell which facilitated the peroxide bonds cleavage, leading high efficiency of ROS generation. The accelerated proton transition was confirmed with AC impedance method, resulting in fast and elevated surface bound Fe 2+ for persulfate decomposition into active species. Furthermore, BZVI@OA/PS system demonstrated high tolerance over wide initial pH range and promising reusability within 6 cycles. This work clarifies an effective strategy for developing efficient modified ZVI as a PS activator for organic pollutant degradation in water.
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高影响因子
SENSORS
·
2021
·Vol. 21
·期 6
·1972
·
IF 3.576
Shidai Tian,Shijie Li,Yijie Hu,Wei Wang,Aifang Yu,Lingyu Wan,Junyi Zhai
There are numerous works that report wirelessly controlling the locomotion of soft robots through a single actuation method of light or magnetism. However, coupling multiple driving modes to improve the mobility of robots is still in its infancy. Here, we present a soft multi-legged millirobot that can move, climb a slope, swim and detect a signal by near-infrared irradiation (NIR) light or magnetic field dual actuation. Due to the design of the feet structure, our soft millirobot incorporates the advantages of a single actuation mode of light or magnetism. Furthermore, it can execute a compulsory exercise to sense a signal and analyze the ambience fluctuation in a narrow place. This work provides a novel alternative for soft robots to achieve multimode actuation and signal sensing.Keywords:soft millirobot;multi-legged;actuator;light-driven;magnetic response
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高影响因子
Nanoscale
·
2021
·Vol. 13
·期 9
·4855-4870
·
IF 7.79
Qifang Chen,Xianbin Ma,Li Xie,Wenjie Chen,Zhigang Xu,Erqun Song,Xiaokang Zhu,Yang Song
Ferroptosis therapy, which applies ferroptotic inducers to produce lethal lipid peroxidation and induce the death of tumor cells, is regarded as a promising therapeutic strategy for cancer treatment. However, there is still a challenge regarding how to increase reactive oxygen species (ROS) accumulation in the tumor microenvironment (TME) to enhance antitumor efficacy. Herein, we designed a nanosystem coated with the FDA approved poly(lactic-co-glycolic acid) (PLGA) containing ferrous ferric oxide (Fe3O4) and chlorin E6 (Ce6) for synergistic ferroptosis-photodynamic anticancer therapy. The Fe3O4-PLGA-Ce6 nanosystem can dissociate in the acidic TME to release ferrous/ferric ions and Ce6. Then, the Fenton reaction between the released ferrous/ferric ions and intracellular excess hydrogen peroxide can occur to produce hydroxyl radicals (˙OH) and induce tumor cell ferroptosis. The released Ce6 can increase the generation and accumulation of ROS under laser irradiation to offer photodynamic therapy, which can boost ferroptosis in 4T1 cells. Moreover, magnetic monodisperse Fe3O4 loading provides excellent T2-weighted magnetic resonance imaging (MRI) properties. The Fe3O4-PLGA-Ce6 nanosystem possesses MRI ability and highly efficient tumor suppression with high biocompatibility in vivo due to the synergism of photodynamic and ferroptosis antitumor therapies.
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Meimei Du,Hainan Kuang,Yongqing Zhang,Xianlin Zeng,Conghao Yi,Imtyaz Hussain,Shaobin Huang,Shuaifei Zhao
Imidacloprid (IMI) removal by persulfate (PS) oxidation activated by ball-milled FeS 2 /Fe0 composite was investigated in terms of reaction conditions and mechanisms. The ball-milled FeS 2 /Fe 0 with a mass ratio of 1:9 exhibited the highest activating efficiency for PS among the investigated mass ratios of 9:1, 4:1, 1:1, 1:4 and 1:9. Increasing dosages of ball-milled FeS 2 /Fe 0 and PS promoted IMI removal. At initial pH of 4.6 and initial IMI concentration of 0.15 mol/L, the optimal dosage of ball-milled FeS 2 /Fe 0 and PS were 0.1 g/L and 2.5 mmol/L, respectively, removing 99.8% of IMI after 60-min reaction. The ball-milled FeS 2 /Fe 0 could also activate PS effectively in a wide pH range from 3 to 9. Characterizations including Scanning electron microscopy with energy dispersive spectroscopy (SEM-EDS) and X-ray photoelectron spectroscopy (XPS) revealed that the high activation efficiency was related to FeS produced on Fe 0 surface. Activation efficiency of PS was enhanced by accelerated electron transfer mediated by increased ferrous species, ultimately, the removal efficiency of IMI was improved. The released Fe 2+ activated PS to generate SO 4 -· and·OH. SO 4 -· was detected to be predominant reactive oxygen species in IMI degradation and three different pathways for IMI degradation were proposed. This study developed a efficient method to activate PS by FeS 2 modify Fe 0 prepared by ball milling a mixture of Fe 0 and FeS 2 , which can provide some new insights into the degradation of organic pollutants .
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危险品化学品经营许可证（带存储）