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Journal of Environmental Chemical Engineering · 2024 · IF 7.4

A novel electrochemical sensor of DNAzyme/AuNPs/Fe/ZIF-8/GCE for Pb2+ detection in the soil solution with enhanced sensitivity, anti-interference and stability

Peipei Song,Zhirui Fan,Shuai Sun,Chengye Sun,Jun Wang

In recent years, lead (Pb) contaminated soil has caused irreversible damage to human beings. It is urgent to develop a novel technology for accurate detection of Pb in the soil solution. Herein, a new electrochemical sensor was fabricated. Fe/ZIF-8 was used as the modification material, gold nanoparticles (AuNPs) were electrodeposited, and DNAzyme was applied on the surface as the probe. Under the optimum conditions (DNAzyme concentration of 1 μmol, fixation time of 4 min, incubation time of 17 h and reaction time of 30 min), the detection range was 5×10 −12 ∼ 5×10 −5 M, and the minimum detection limit was 10 −13 M (3δ). Furthermore, the electrochemical sensor demonstrated outstanding anti-interference ability to common cations, anions, organic compounds and other interference factors. After four consecutive tests, the relative standard deviation (RSD) was only 0.39%, and it still displayed excellent reproducibility with 0.69% of RSD. After 20 days, the sensor’s response to Pb 2+ remained at 93.58%. In addition, the sensor could accurately detect Pb 2+ in the actual soil solutions, and the recoveries of the samples ranged from 92% to 109.4%. In conclusion, this electrochemical sensor can specifically detect Pb 2+ in the soil solution with enhanced sensitivity, anti-interference capability and stability, which is of great significance for Pb 2+ detection in the field.

研究领域: 环境科学 · 分析化学 · 纳米技术
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JOURNAL OF ALLOYS AND COMPOUNDS · 2020 · IF 4.65

Facile synthesis of structurally ordered low-Pt-loading Pd–Pt–Fe nanoalloys with enhanced electrocatalytic performance for oxygen reduction reaction

Yingfang Zhu,Sihao Wang,Qingyu Luo,Haifu Huang,Shaolong Tang,Youwei Du

Developing electrocatalysts with high-Pt-utilization efficiency and appropriate surface oxygen affinity through a facile and scalable route is urgently needed for proton exchange membrane fuel cells. Here, SPD-annealing strategy is demonstrated to prepare ordered low-Pt-loading Pd–Pt–Fe nanoalloys with an average particle size of less than 5 nm and excellent electrocatalytic performance. Furthermore, the ORR performances of Pd–Pt–Fe/C nanoalloy catalysts are rationally modified by means of both precise composition control and structural transformation. With an optimal component proportion, the prepared Pd 0 . 75 Pt 0 . 25 Fe/C catalyst exhibits the most excellent intrinsic activity due to the synergistic interaction of lattice strain and ligand effect. Benefiting from the compressive strain effect induced by the relatively tight arrangement of the ordered structure, the adsorption energy of the intermediate oxygen-containing species is effectively weakened, enabling the Pd 0 . 75 Pt 0 . 25 Fe/C to obtain enhanced ORR catalytic performance in acidic condition. Notably, compared with the disordered Pd 0 . 75 Pt 0 . 25 Fe/C, the ordered Pd 0 . 75 Pt 0 . 25 Fe/C shows an extremely superior stability of 98.5% mass activity retention after 10 000 cycles. This work could provide a facile and versatile approach to constructing the ordered low-platinum electrocatalysts with enhanced ORR properties.

研究领域: 材料科学 · 电化学 · 能源科学
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JOURNAL OF HAZARDOUS MATERIALS · 2019 · IF 7.65

Multiple bimetallic (Al-La or Fe-La) hydroxides embedded in cellulose/graphene hybrids for uptake of fluoride with phosphate surroundings

Yali Guo,Xu Xing,Yanan Shang,Baoyu Gao,Lei Zhang,Qinyan Yue,Li Qian,Zihang Wang

To insight into the selective adsorption mechanism of fluoride in the bimetallic system, Fe-La or Al-La composites were comparatively embedded onto the cellulose/graphene hybrids (CG hybrids) to fabricate the Fe-La@CG hybrids or Al-La@CG hybrids for fluoride uptake with existing phosphate. The results showed that Al-La@CG hybrids were mainly in the amorphous nature, while Fe-La@CG hybrids have the identical diffraction peaks as compared with those of hydrated lanthanum oxides (HLO) and hydrated iron oxides (HFO). Fluoride capture by Al-La@CG and Fe-La@CG hybrids followed the similar tendencies with the pH altering, but the adsorption performance of Al-La@CG hybrids was better than that of Fe-La@CG hybrids at the same pH levels. Adsorption of fluoride onto Al-La@CG hybrids exhibited less sensitivity and high selectivity with existing phosphate as compared with that of Fe-La@CG hybrids, which further indicated that the Al-La@CG hybrids were more preferable for fluoride adsorption. The fraction areas of La-F and Al-F accounted for 79.1 % and 20.9%, which indicated that the fluoride onto the Al-La@CG hybrids was mainly based on the La species. Similarly, La-F in exhausted Fe-La@CG hybrids accounted for 55.6%, higher than that (44.4%) of Fe-F.

研究领域: 材料科学 · 环境科学
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DESALINATION · 2024 · IF 8.3

Long-term and efficient treatment of shale gas flowback wastewater by the novel double SEP@Fe-Mn/RGO composite membranes method

Xuehan Xiao,Zongxue Yu,Juan Wang,Shiyi Luo,Yan Huang,Dingmei Han,Junchen Li,Zhiquan Chen,Jie Wang,Minggang Huang

The long-term and efficient treatment of shale gas wastewater is an inevitable tendency. This study employed the SEP@Fe-Mn/RGO composite membrane series for the membrane separation treatment of shale gas wastewater. Different proportions and different function of SEP@Fe-Mn/RGO composite membranes were obtained through the method of electrostatic self-assembly. This study researched the “Trade-off” issue of membranes separation through the analysis,resulting in membranes that best meets the separation requirements for shale gas wastewater. After two membrane separation, The oil-water separation efficiency (COD 2040 mg/L and TOC 487.14 mg/L) of shale gas wastewater was >99.3 %. The removal rate of the main salt component (Na 2 SO 4 ) reached 83.56 %, and the removal rate of major heavy metal ions (Fe 3+ , Cr 3+ , Ba 2+ ) was above 60 %. Because of the continuous generation of in-situ bubbles by the reaction of MnO 2 with H 2 O 2 , and Fenton reactions on the membrane, which further accelerated the separation of pollutants. In a variety of harsh water environments, this membrane series remained stable within 12 h. Simple to prepare, cost-effective, low in energy consumption, and environmentally friendly, which makes it promising for wide applications in the field of petroleum water treatment.

研究领域: 环境科学 · 材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Achieving a “all in one” Fe/Tm-MOFs with controllable photothermal and catalytic performance for imaging-guided multi-modal synergetic therapy

Haiqing Gao,Qin Ji,Bin Chi,Caixue Lin,Gang Ding,Yingxi Wang,Xiaolan Yu,Zushun Xu,Run Zhang,Ling Li,Jing Wang

Targeting excess H 2 O 2 in the tumor microenvironment, nanotheranostic agents for catalytic therapy are designed based on Fenton reaction, catalyzing H 2 O 2 into oxygen and hydroxyl radical ( OH). But the catalytic efficiency in tumor microenvironment is not satisfactory. In order to solve the problem, a series of bimetallic-dual ligands metal-organic frameworks Fe/Tm-MOFs were designed, that Fe 3+ and Tm 3+ as metalions, 2-methylimidazole and trimesic acid as ligands. Due to the doped Tm 3+ in Fe/Tm-MOFs and the conjugated structures formed by two ligands, the rate of electron transfer was improved, thus promoting the generation of OH at some extent. In addition, the photothermal effect of Fe/Tm-MOFs further promotes the generation of OH, which was evidenced by the 3,3′,5,5′-tetramethylbenzidine(TMB). Combining the drug loading and release capabilities of Fe/Tm-MOFs, synergetic therapy of photothermal/chemo-/catalytic therapy can be achieved. In vitro results reveal that DOX release behaviors are both pH- and thermal-responsive. In vivo anti-cancer results show that the tumors of mice almost disappeared within 10 days, which were injected with Fe/Tm-MOFs/DOX and irradiated with 808 nm for 10 min. Thus, an excellent therapeutic performance has been achieved. Besides, Fe/Tm-MOFs can serve as a multimodality bioimaging contrast agent, covering fluorescence imaging, photothermal imaging and magnetic resonance imaging. Thus, an all-in-one nanotheranostic agent is constructed, improving the catalytic efficiency and providing a novel method to design an efficient nanotheranostic agent.

研究领域: 生物医学工程 · 纳米医学 · 肿瘤学
✓ 已验证 DOI PubMed 高影响因子
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JOURNAL OF ALLOYS AND COMPOUNDS · 2021 · IF 5.316

Fe–Nx–C sites decorated porous carbon nanorods with huge specific surface area boost oxygen reduction catalysis for Zn-air batteries

Lei Cao,Maliang Zhang,Kunmei Su,Feng Gu,Zhenhuan Li

Decorating porous carbon nanomaterials with rich homodispersed metal cluster and heteroatoms can effectively shorten the diffusion pathway of oxygen and expose more active sites, thereby promoting oxygen reduction reaction (ORR). Herein, hierarchical porous carbon nanorods with homodispersed Fe–N x –C active sites are obtained by calcination , etching and ammonia activation of Fe-nitrogenous acid (NTA) coordination polymer nanowires. The obtained Fe-PCNRs-700 as ORR catalysts show the excellent activity with half wave potential (E 1/2 ) of 0.71 V vs. reversible hydrogen electrode (RHE) in 0.5 M H 2 SO 4 and 0.87 V vs. RHE in 0.1 M KOH electrolyte, which owe to its huge specific surface area (1652 m 2 g −1 ), hierarchical pore structure , homodispersed Fe–N x –C active sites and structural defects. Furthermore, using Fe-PCNRs-700 as a cathode catalyst in both liquid and flexible solid Zn-air batteries, and the assembled liquid batteries display the high power density of 161 mW cm −2 and robust charge/discharge stability of 116 h.

研究领域: 材料科学 · 电化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF POWER SOURCES · 2025 · IF 7.9

Study on the formation mechanism of self-assembly bamboo-shaped carbon nanotubes enriched with highly stable Fe-N4 sites for Zn-air batteries

Lihui Xiao,Yaqiang Li,Peixia Yang,Qiang Lv,Xiangyu Lu,Hao Xu,Ruopeng Li,Huiling Zhang,Shengbo Yang,Anmin Liu,Dan Wang,Jinqiu Zhang,Maozhong An

Carbon nanotubes' (CNTs) preparation and formation mechanisms are of great interest. To improve their performance in the oxygen reduction reaction (ORR), a post-treatment to add active centers is required. This study presents a simple method using a molten-salt template to self-assemble bamboo-shaped CNTs (B-Fe-N-C) with highly stable Fe-N 4 (Fe-pyridinic-N 4 ) sites. By analyzing the evolution of high-temperature materials and the intermolecular bonding process, the formation mechanism of B-Fe-N-C follows a two-dimensional material synthesis--bonding--self-assembly--growth mechanism. Impressively, B-Fe-N-C exhibits superior ORR performance (a half-wave potential of 0.868 V) and stability (only 3 mV attenuation after 10000 cycles of accelerated durability test) in alkaline medium. Density functional theory calculations demonstrate that Fe-Pyridinic-N 4 sites can lower the energy barrier for ORR. Furthermore, Comsol multiphysics simulations confirm the significant enhancement of oxygen mass transfer by bamboo-shaped B-Fe-N-C. Therefore, B-Fe-N-C is employed in zinc-air batteries, resulting in nice discharge performance and high peak power density.

CAS / MDL: 13478-10-9 7647-14-5
研究领域: 材料科学 · 电化学 · 理论计算
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2021 · IF 8.128

Phenanthroline bridging graphitic carbon nitride framework and Fe (II) ions to promote transfer of photogenerated electrons for selective photocatalytic reduction of Nitrophenols

Ying Liu,Yi Liu,Yingying Xu,Qingshen He,Rongyang Yin,Pengfei Sun,Xiaoping Dong

Nitrophenols (NPs) are widely used in industries and highly toxic to ecological environment and human health. Because aminophenols (APs) are important chemicals, catalytic reduction of NPs via efficient and environment-friendly strategies is of great importance. Herein, we developed a green photocatalysis route to efficiently convert NPs to APs using a Fe (II) modified graphitic carbon nitride (g-C 3 N 4 ) photocatalyst, where phenanthroline units were employed to bridge Fe (II) and carbon nitride framework. The optimized sample P-CN-8-Fe presented significantly improved absorption of visible light, separation of photogenerated charges and carrier transportation in comparison with the pristine g-C 3 N 4 and the modified samples of CN-Fe and P-CN-8. Accordingly, the P-CN-8-Fe showed a high conversion (97%) of p -nitrophenol ( p -NP) to p -aminophenol ( p -AP) under 2 h visible light irradiation, and meanwhile possessed high photocatalytic durability. Its high activity was also demonstrated through photocatalytic reduction of other NPs and nitrobenzene compounds. Finally, a possible mechanism was proposed for the photocatalytic reduction of p -NP by P-CN-8-Fe. This work provides an effective approach to prepare Fe (II) modified g-C 3 N 4 through the bridging effect of phenanthroline group, which is a potential visible light driven photocatalyst for reduction of nitrobenzene derivatives.

研究领域: 环境科学 · 材料科学
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Materials Science and Engineering B-Advanced Functional Solid-State Materials · 2025 · IF 4.6

Highly stable and efficient catalyst fabricated with in situ exsolved Co-Fe bimetallic nanoparticles anchored on (Ba0.9K0.1)0.9Co0.5Fe0.4Nb0.1O3-δ for CO2 electrolysis

Yangyang Zhao,Haowei Li,Xiaoyu Wang,Tao Cong,Yijian Wang,Hesheng Zheng,Zhongyi Zhao,Xingchen Feng,Juntao Feng,Pei Wang,Kai Yang,Xifeng Ding

Solid oxide electrolysis cells (SOECs), featuring high current density and Faradaic efficiency, have been extensively recognized for CO 2 electrolysis abilities. However, it is a challenge to find high performance electrode materials with excellent catalytic activity and preferable stability. Herin, hetero-structured perovskite with exsolved Co-Fe nanoparticles is developed via in - situ reduction of the (Ba 0.9 K 0.1 ) 0.9 Co 0.5 Fe 0.4 Nb 0.1 O 3- δ ((BK) 0.9 CFNb). The corresponding SOEC R-(BK) 0.9 CFNb/LSGM/LSCF achieves excellent electrochemical performance with a current density of 0.813 A cm −2 at 1.5 V and 800 °C, which is 30 % higher than the counterpart with untreated (BK) 0.9 CFNb cathode. Its high catalytic activity is attributed to electron feeding effect of in situ exsolved Co-Fe nanoparticles and enhanced CO 2 adsorption with high concentration of oxygen vacancies in perovskite substrate surface. Moreover, the R-(BK) 0.9 CFNb-cell shows much better stability than parent (BK) 0.9 CFNb-cell, which is ascribed to the structural anchoring of the alloy nanoparticles. This study provide an attractive strategy for the future development of SOECs.

研究领域: 材料科学 · 能源化学
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CHEMICAL ENGINEERING SCIENCE · 2023 · IF 4.7

Metal-organic framework-derived Fe/Fe3C embedded in N-doped carbon as a highly efficient oxygen reduction catalyst for microbial fuel cells

Shuting Huang,Yanxian Geng,Dongyun Chen,Najun Li,Qingfeng Xu,Hua Li,Jianmei Lu

Microbial fuel cells (MFCs) have become new energy approach for sustainable development. The exploitation of economic and efficient electrocatalysts for the oxygen reduction reaction (ORR) is essential for obtaining remarkable MFCs performance. Herein, metal–organic framework (MOF)-derived Fe/Fe 3 C embedded in nitrogen-doped carbon hybrids, prepared through a simple solvothermal and pyrolysis approach, are highly efficient ORR catalysts. The unique mixed dimension (1D/2D) and mesoporous structure provide abundant active sites and build transfer channels for improvement. Additionally, the presence of nitrogen doping played an important role to accelerate electron diffusion and transport. A maximum power density of 1974.75 ± 26.16 mW m −2 is earned by Fe/Fe 3 C/NC-800, and is 1.45 times of 20% Pt/C (1366.45 ± 28.65 mW m −2 ). Therefore, the Fe/Fe 3 C/NC catalyst is a prospective ORR catalyst in MFCs and in future renewable energy storage and conversion technologies.

研究领域: 材料科学 · 能源技术 · 环境科学
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Environmental Science-Nano · 2020 ·Vol. 7 ·期 12 ·3814-3823 · IF 7.683

In situ controlled synthesis of porous Fe–N–C materials from oily sludge by chlorinating calcination and their novel application in supercapacitors

Hanfeng Zhou,Zhibo Deng,Tianbao Liu,Tao Liu,Lijuan Zhang,Xintai Su,Zhang Lin

The science linking thermochemical conversion of large-scale industry oily sludge with applied materials has been improved in the last ten years. However, with the traditional converting methods it is hard to precisely control the composition and structure of oily sludge-based products during pyrolysis due to the complexity of the composition of the oily sludge. Here, a chlorinating calcination method using sodium chloride (NaCl) as a chlorinating salt and template was first developed to prepare porous Fe–N–C materials (FCN-500) through pyrolysis of oily sludge containing iron-bearing minerals and pyridine. The formation mechanism of FCN-500 was proposed, where iron ions (Fe3+) from the inorganic component (anorthite) in the sludge were rapidly dissociated with the assistance of NaCl, followed by coordination with the organic component (pyridine nitrogen) in the oily sludge to form the pyridine nitrogen–iron ((C5H6N)n–Fe) complex, and then carbonization. As-obtained FCN-500 exhibited higher specific capacitance (286.3 F g−1 at a current density of 0.5 A g−1), enhanced energy density (33.5 W h kg−1 at a power density of 606.1 W kg−1) and more excellent stability and durability (more than 80.1% capacitance retention after 10 000 cycles) compared with two other electrodes. The reasonably better performance of the obtained FCN-500 in supercapacitors (SCs) is attributed to its large surface area, hierarchically porous channels, high conductivity, and unique Fe–N–C structure. Therefore, this work not only provides a feasible way to solve the bottleneck problem in sludge pyrolysis, but also provides a method to design large scale porous Fe–N–C materials for practical applications.

研究领域: 环境科学 · 材料科学 · 能源科学
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Industrial Chemistry & Materials · 2024 · IF 0

Elongated Fe–N–C containing trace atomic Co dopants for high power density PEMFCs

Jiayao Cui,Junyong Min,Hao Wang,Jianglan Shui,Lishan Peng,Zhenye Kang,Jieyuan Liu,Qingjun Chen,Shuo Bai,Yanrong Liu

Developing single-atom Fe–N4/C catalysts is crucial for the large-scale implementation of proton exchange membrane fuel cells (PEMFCs). While Fe–N4/C catalysts are inherently active in accelerating the slow ORR process, their performance is still inferior to that of Pt/C. Herein, a trace Co-doped Fe single-atom catalyst (Fe(tCo)–N–C) containing more active Fe2N8 sites has been synthesized. Interestingly, compared with typical FeN4 sites in an Fe–N–C electrocatalyst, the Fe2N8 sites generate a larger Fe–N bond length due to Co-doping. The elongated Fe–N bond in Fe2N8 lowers the d-band center and charge density of iron sites, enhancing the ORR process by facilitating the formation of *OOH and generation and desorption of *OH. Fe(tCo)–N–C manifested excellent acidic and alkaline ORR activity, with a half-wave potential (E1/2) of 0.80 V in HClO4 solution and 0.89 V in KOH medium. More importantly, high peak power densities (Pmax) were realized by applying Fe(tCo)–N–C in PEMFCs, with the Pmax reaching 890 mW cm−2 in H2–O2 and 380 mW cm−2 in H2–air. Additionally, trace Co dopants in the catalyst improved carbon graphitization and provided high ORR catalytic stability. This research introduces an innovative approach to engineering highly active Fe2N8 sites, providing valuable insights for the sustainable progress of PEMFC technology.

研究领域: 电化学 · 催化 · 能源材料 · 燃料电池 · 纳米技术
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