查找使用阿拉丁产品的科研文献

Optimizing the thiosulfate-mediated zerovalent iron/persulfate activation systems: Trade-off between Fe(III)/Fe(II) cycling and quenching effects in environmental remediation

Maolin Wang,Mi Deng,Gang Zhao,Yanchun Fan,Tianwen Liu,Ying Huang,Lan Peng,Haoyang Fu,Shengqiong Fang

The remediation of organic-contaminated water is a critical environmental challenge, and iron-based persulfate (PS) activation processes have emerged as a promising solution. However, the introduction of reductive sulfur species, while accelerating the Fe(III)/Fe(II) redox cycle, may also quench reactive species, potentially compromising the efficiency of Fenton-like systems. Here we systematically investigate the trade-off between accelerated Fe(III)/Fe(II) cycling and quenching effects in the zerovalent iron/PS (ZVI/PS) system using thiosulfate (TSF) as an activator. Our results show that low-level TSF (0.03–1.00 mmol/L) effectively facilitated the removal of naphthalene (Nap) and atrazine (ATZ), respectively. This enhancement is attributed to accelerated ZVI dissolution and FeS x formation, which promote the Fe(III)/Fe(II) cycle, with Fe(IV) was identified as the primary active species. However, high-level TSF (>1.0 mmol/L) drastically reduced Nap removal due to PS consumption and active species elimination. The optimal TSF dosage of 0.20 mmol/L (TSF/PS molar ratio of 1:10) demonstrated robust organic pollutant degradation, achieving a 22-fold increase in the rate constant ( k obs ) for Nap removal and 0.47–7.5-fold increases for ATZ removal. These findings highlight the potential of the TSF-ZVI/PS system as a versatile and efficient solution for degrading a wide range of organic pollutants, including PAHs and herbicides, in water treatment applications.

Doubled Capacity and Cyclability of Berlin Green Cathodes with Low-Spin Fe Activation and NH4+ Co-Insertion for Rocking-Chair Fe-Ion Batteries

Xiang Ji,Yi Li,Yanlong Wang,Jian Jiang,Maowen Xu,Jianhui Zhu

Rechargeable Fe-ion batteries with overwhelming cost/environmental benign superiorities hold great promise in large-scale charge-storage applications. However, there is still a lack of competitive cathodes with prominent capacity and long-term cyclability. To overcome these constraints, a unique Fe 2+ /NH 4 + co-insertion strategy is proposed, enabling both doubled reversible capacity and cyclic life of Berlin green (FeHCF) cathodes. The Fe 2+ insertion proves to induce FeHCF lattice contractions, alter ligand environment/activation energies of low-spin Fe III, and hence boost the redox conversion depth, while NH 4 + co-insertions help to elevate the cathode capacities by utilizing Fe 2+ -unoccupied reaction sites. Besides, they generate hydrogen bonds between inserted NH 4 + ions and N atoms in FeHCF, capable of vastly strengthening the cathode's cyclic durability. Cathodes in such collaborative dual-cation electrolytes exhibit a remarkable capacity of 162 mAh g −1 (4 A g −1 ) and far prolonged operation lifespan (over 1000 cycles) when compared to single-cation cases. The assembled full cells demonstrate impressive energy densities up to 70.4 Wh kg −1 , and far superior capacity retention of 88% after all the cycling. This work may offer a simple/feasible, and effective route to render high-capacity and long-lasting cathodes for future/practical Fe-ion battery systems.

Thermo-Electro-Magnetic Interactions and ≈1 nm Fe Interfacial Layer Realize High Average ZT in Fe/Mg3(Sb,Bi)2 Below 300 °C

Kangpeng Jin,Haonan Nie,Fengxian Gao,Jiang-Jiang Ma,Mingfang Shu,Xi Yan,Zhen-Hua Ge,Xiao Gao,Weiyun Zhao,Ming Liu,Yuan Yu,Jie Ma,Biao Xu,Liangwei Fu

Mg 3 (Sb,Bi) 2 alloys offer exceptional near-room temperature thermoelectric (TE) performance comparable to Bi 2 Te 3 . However, the low carrier mobility due to Mg vacancies and relatively high lattice thermal conductivity adversely affect overall TE performance. Herein, carrier mobility and thermal conductivity of Mg 3 (Sb,Bi) 2 are decoupled by modulating both the phase interface and grain boundaries through incorporating different sizes of iron (Fe). Ferromagnetic micrometer-sized Fe particles enhance the figure of merit ( ZT ) more than superparamagnetic nano-sized counterparts. Magnetic moments of Fe induce the charge density overlap near phase boundaries and ≈1 nm Fe interfacial layer lowers grain-boundary barriers, leading to sharply increased carrier mobility. Moreover, the additional magnon-phonon scattering reduces lattice thermal conductivity by over 40%. Consequently, Fe/Mg 3 (Sb,Bi) 2 composite achieves a high average ZT of 1.4 over room temperature to 573 K. The fabricated Mg 3 (Sb,Bi) 2 -CdSb module demonstrates a high conversion efficiency of 8.4% under a 275 K temperature gradient, among the best for Mg 3 (Sb,Bi) 2 -based modules. This work uncovers the role of thermo-electro-magnetic interactions in bolstering TE performance and inspires the development of low-cost, high-efficiency TE modules for low-grade heat recovery.

Biomass Cellulose-Derived Carbon Aerogel Supported Magnetite-Copper Bimetallic Heterogeneous Fenton-like Catalyst Towards the Boosting Redox Cycle of ≡Fe(III)/≡Fe(II)

Qiang Zhao,Jiawei Yang,Jiayi Xia,Gaotian Zhao,Yida Yang,Zongwei Zhang,Jing Li,Fang Wei,Weiguo Song

To degrade high-concentration and toxic organic effluents, we developed Fe-Cu active sites loaded on biomass-source carbon aerogel (CA) to produce a low-cost and high-efficiency magnetic Fenton-like catalyst for the catalytic oxidative decomposition of organic pollutants. It exhibits excellent performance in catalytic Fenton-like reactions for RhB removal at an ultrahigh initial concentration of up to 1000 ppm. To be specific, Fe3O4and Cu nanoparticles are generated in situ on a mesoporous CA support, denoted as an Fe3O4-Cu/CA catalyst. Experimentally, factors including initial dye concentration, catalyst dosage, H2O2dosage, pH, and temperature, which significantly influence the oxidative degradation rate of RhB, are carefully studied. The RhB (1000 ppm) degradation ratio reaches 93.7% within 60 min under low catalyst and H2O2dosage. The catalyst also shows slight metal leaching (almost 1.4% of total Fe and 4.0% of total Cu leached after a complete degradation of 25 μmol RhB under conditions of 15 mg catalyst dosage, 20 mL RhB solution (600 ppm), and 200 μL 30 wt% H2O2dosage, at pH of 2.5, at 40 °C), good catalytic activity for degrading organic pollutants, excellent reusability, and good catalytic stability (the degradation ratio is nearly 82.95% in the 8th cycle reaction). The synergistic effect between Fe and Cu species plays a vital role in promoting the redox cycle of Fe(III)/Fe(II) and enhancing the generation of ·OH. It is suitable for ultrahigh-concentration organic pollutant degradation in practical wastewater treatment applications.

Ligase chain reaction-based electrochemical biosensor for the ultrasensitive and specific detection of single nucleotide polymorphisms

Wancun Zhang,Fang Hu,Xianwei Zhang,Wei Meng,Yaodong Zhang,Yinsen Song,Huanmin Wang,Peng Wang,Yueqing Gu

In this study, a simple, robust, label-free electrochemical biosensor based on the ligase chain reaction (LCR) was developed for the highly sensitive and selective detection of single nucleotide polymorphisms (SNPs) using Fe(CN)63−/Fe(CN)64− as a redox indicator. High sensitivity and specificity were achieved by using the LCR, which employs a thermostable and single-base discerning Hifi Taq DNA ligase to repeatedly ligate adjacently hybridized LCR-specific probes during thermal cycles, resulting in the highly specific exponential amplification of DNA targets. The electrochemical signal of the biosensor was further decreased using stem-loop probe DNA (SL-DNA), which specifically hybridized with LCR products on the electrodes. The linear dynamic range and high sensitivity of the mutant DNA (MutDNA) and wild-type DNA (WtDNA) LCR-based electrochemical biosensors for the detection of MutDNA and WtDNA were studied in vitro, with a broad linear dynamic range of 10 aM to 10 pM and detection limits of 1.18 aM and 0.35 aM, respectively. In addition, the MutDNA and WtDNA LCR-based electrochemical biosensors were able to accurately detect allele frequency changes as low as 0.1%. In summary, the developed LCR-based electrochemical biosensor provides a useful platform to monitor SNPs in a highly sensitive and specific manner.

Mesoporous Carbon as Galvanic-Corrosion Activator Accelerates Fe Degradation

Cijun Shuai,Yulong Li,Fang Deng,Youwen Yang,Shuping Peng,Fangwei Qi,Lida Shen

Iron (Fe) has attracted intensive attention as a bone implant material because of its inherent biodegradability, favorable biocompatibility and mechanical properties. Nevertheless, it degrades too slowly in a physiological environment, which limits its further clinical application. In this work, mesoporous carbon (MC) was introduced into Fe bone implant manufactured via a laser-additive manufacturing process. Particularly, MC possesses a noble standard corrosion potential and excellent electrical conductivity, thus acting as an effective cathode and activating micro-galvanic corrosion in the Fe matrix. More importantly, its high specific surface area enhanced the area ratio between cathode and anode, which further enhanced the galvanic corrosion effect. As a consequence, the corrosion rate was enhanced from 0.09 to 0.24 mm/year based on immersion tests. Besides, Fe/MC composite exhibited good cytocompatibility, as well as excellent mechanical properties. The positive results proved that the Fe/MC composite shows great potential as a bone implant.

Amorphous Co–Fe–P nanospheres for efficient water oxidation

Tanyuan Wang,Chao Wang,Yue Jin,Anna Sviripa,Jiashun Liang,Jiantao Han,Yunhui Huang,Qing Li,Gang Wu

Transition metal phosphides are often studied as hydrogen evolution reaction cathode catalysts, but scarcely as oxygen evolution reaction (OER) anode catalysts for water oxidation. Herein, we report a new amorphous Co0.63Fe0.21P0.16 OER catalyst, which was prepared through a one-step solvothermal process. This catalyst exhibits extraordinary OER catalytic activity in alkaline media and is superior to the state of the art IrO2 in 1.0 M KOH, capable of yielding a current density of 10 mA cm−2 at an overpotential of only 217 mV. This newly achieved high activity outperforms most reported transition metal phosphide catalysts. During the OER, the surface layers of the Co0.63Fe0.21P0.16 nanospheres (200–500 nm) are oxidized, which show the typical Tafel slope of oxides around 40 mV dec−1. The in situ formation of surface Co oxides in the catalysts during the OER along with an optimal doping of Fe are found to be crucial for their remarkable activity. In particular, the metal-rich amorphous phosphide cores, i.e., substrates, probably contribute to OER performance of the catalysts due to their high electrical conductivity. This new type of surface oxidized amorphous transition metal phosphide would provide a new pathway for the design of high-performance OER electrocatalysts.

Degradation of diclofenac by Fe(II)-activated peracetic acid

Zhenran Wang,Hongle Shi,Shixiang Wang,Yiqing Liu,Yongsheng Fu

Dual-Responsive Triple-Synergistic Fe-MOF for Tumor Theranostics

Zhiwei Chen,Yaoji Sun,Jiawei Wang,Xi Zhou,Xiangjian Kong,Jiashen Meng,Xingcai Zhang

The intelligent responsive drug delivery system has great application potential in cancer precision therapy. Although many antitumor methods have been developed based on drug delivery systems, most of them yet suffer from poor antitumor efficiency. In this project, a near-infrared and pH dual-response multimodal collaborative platform for diagnosis and treatment (PCN-DOX@PDA) was constructed. We used PCN-600 as a vehicle loaded with antineoplastic drugs and polydopamine (PDA). Under 633 nm laser irradiation, the ligand tetrakis(4-carboxyphenyl)porphyrin (TCPP) in PCN-600 can generate singlet oxygen (1O2) and kill tumor cells. PDA is used as photothermal agent of PTT. PCN-DOX@PDA achieves the intelligent release of antitumor drugs by responding to the weak acidity of the tumor microenvironment and thermal stimulation generated by NIR irradiation. In addition, since the central ion of PCN is Fe3+, PCN-DOX@PDA realizes the diagnosis and treatment of tumors through magnetic resonance imaging-mediated tumor chemotherapy and photothermal and photodynamic synergistic therapy. This triple synergistic strategy showed excellent biocompatibility and antitumor ability in in vivo experiments on a 4T1 tumor-bearing mouse model, indicating that PCN-DOX@PDA has a good development prospect in the field of precision cancer therapy and diversified biomedical applications.

Carbon-covered Fe-pillared bentonite electrode boosting capacitive deionization

Yue Zhu,Hao Wang,Boshuang Zhang,Bin Hu,Yiwen Wang,Meng Li,Jianmao Yang,Jianyun Liu

Capacitive deionization (CDI), as an energy-efficient desalination technique, has attracted worldwide attention. Bentonite , a natural clay with 2-dimensional structure, is much popular for water treatment because of its high adsorption capacity , low cost and environmental benign properties. However, the poor conductivity and narrow interlamellar spacing limit its electrochemical application. In this work, a carbon-covered Fe-pillared bentonite (PILB@C) was fabricated as a new type of electrode materials for CDI. Through Fe-pillaring in bentonite, the interlayer spacing enlarged, accompanied with enhanced specific surface areas and abundant mesopores . The further carbon coating endowed the bentonite with good conductivity and facilitating ion-transportation. The dual-regulated composites possessed the negatively charged surface feature, favorable for inverted capacitive deionization (i-CDI) with improved deionization performance. Under the optimal carbon loading, the PILB@C electrode delivered a superior desalination capacity (16.23 mg g −1 , in 10 mM NaCl). Because of the intrinsic structural stability of bentonite, the desalination system exhibited the excellent cycling stability (90 % capacity retention over 50 cycles). When applied for industrial and domestic water purification , the PILB@C electrode realized salinity reduction and de-mineralization. This natural bentonite is nontoxic and cheap, rendering it highly promising as an electrode material candidate for future water treatment.

EFFICIENT REMOVAL OF NORFLOXACIN FROM WATER BY Fe-MOFs

Wei Fuhua,Ren Qinhui,Wang Nannan,Chen Hongliang,Zhang Yutao,Liang Zhao

The synthesis of Fe-MOFs (metal-organic frameworks) was conducted using a solution heat method, followed by characterization through XRD (X-ray diffraction), SEM (scanning electron microscopy), and TG (thermogravimetry) analysis techniques. Subsequently, the Fe-MOFs were employed for norfloxacin removal. The experimental findings demonstrate that theoretical simulations of norfloxacin adsorption by Fe-MOFs involved the application of pseudo-first kinetic model, pseudo-second kinetic model, and adsorption isotherm. Chemisorption was identified as the primary mechanism observed. Notably, a maximum adsorption capacity of 197.7 mg g-1 was achieved at pH 10. These results underscore the practical feasibility of utilizing Fe-MOFs in applications related to norfloxacin adsorption.

Ferromagnetic Fe-TiO2 spin catalysts for enhanced ammonia electrosynthesis

Wang Jingnan,Zhao Kaiheng,Yao Yongbin,Xue Fan,Lu Fei,Yan Wensheng,Yuan Fangli,Wang Xi

Magnetic field effects (MFE) of ferromagnetic spin electrocatalysts have attracted significant attention due to their potential to enhance catalytic activity under an external magnetic field. However, no ferromagnetic spin catalysts have demonstrated MFE in the electrocatalytic reduction of nitrate for ammonia (NO 3 RR), a pioneering approach towards NH 3 production involving the conversion from diamagnetic NO 3 − to paramagnetic NO. Here, we report the ferromagnetic Fe-TiO 2 to investigate MFE on NO 3 RR. Fe-TiO 2 possesses a high density of atomically dispersed Fe sites and exhibits an intermediate-spin state, resulting in magnetic ordering through ferromagnetism. Assisted by a magnetic field, Fe-TiO 2 achieves a Faradaic efficiency (FE) of up to 97% and an NH 3 yield of 24.69 mg mg cat − 1 at −0.5 V versus reversible hydrogen electrode. Compared to conditions without an external magnetic field, the FE and NH 3 yield for Fe-TiO 2 under an external magnetic field is increased by ~21.8% and ~ 3.1 times, respectively. In-situ characterization and theoretical calculations show that spin polarization enhances the critical step of NO hydrogenation to NOH by optimizing electron transfer pathways between Fe and NO, significantly boosting NO 3 RR activity.