MICROPOROUS AND MESOPOROUS MATERIALS
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2024
·
IF 4.8
Mengting Xu,Zeyu Chen,Yeyang Ni,Wanyong Yang,Xihua Xu,Qing Liu,Zhaoyang Fei,Mifen Cui,Xu Qiao
MIL-126(Fe) shows great potential for aqueous phase drug adsorption due to its permanent porosity and easy modification. Herein, we utilized the ligand installation method to introduce two ligands, 2-amino terephthalic acid (NH 2 -BDC) and 2-nitro terephthalic acid (NO 2 -BDC), into MIL-126(Fe) to prepare MIL-126(Fe)-NH 2 and MIL-126(Fe)-NO 2 , respectively. Various analytical tools were used to confirm the successful installation of the 1, 4-phthalic acid (BDC) series of ligands, as well as the successful introduction of amino (-NH 2 ) and nitro (-NO 2 ) groups. The presence of both -NH 2 and -NO 2 groups improved the adsorption of TC by the adsorbent material, with -NH 2 groups having a stronger influence on the enhancement. The experimental results indicated that MIL-126(Fe)-NH 2 had the highest adsorption performance at the optimal pH of 7, achieving a static adsorption capacity of 326.5 mg/g, which was about twice the adsorption capacity of the original MIL-126(Fe). X-ray photoelectron spectroscopy (XPS) determined that the adsorption of TC by MIL-126(Fe)-NH 2 relies mainly on π-π interaction and Fe-N coordination bonds. Furthermore, the higher adsorption capacity of MIL-126(Fe)-NH 2 can be attributed to the O-H⋯N hydrogen bonds interaction between -NH 2 and the phenolic hydroxyl group (Ph-OH) in the TC molecule.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Hui Li,Xinlei Ren,Wenxue Pan,Shiting Zhu,Jin Zhang,Zhiyuan Yang,Liu Qian,Yueying Wang,Yujing Huang,Lin Guo,Minghui Xiang
The reasonable control of the structure of metal–organic frameworks (MOFs) is a promising strategy for improving their peroxymonosulfate (PMS) activation activity. In this study, ZIF-67 @ZIF-8 was used as a template to prepare bimetallic core–shell Co-Fe@NC via Fe doping and high-temperature carbonization . Co-Fe@NC maintained the core–shell structure of the original MOF, in which cobalt was uniformly distributed in the nitrogen-doped graphite carbon skeleton and the surface of the graphite carbon skeleton was covered with iron. With the synergistic effect of the nitrogen-doped graphite carbon skeleton, iron, and cobalt, 100% of tetrabromobisphenol S (TBBPS) was removed in 60 min with k obs = 0.062 min −1 in Co-Fe@NC-0.2/PMS system. The addition of iron increased the graphitization degree with I D /I G value increased from 0.98 (Co@NC) to 1.034 (Co-Fe@NC-0.2) and electron transfer rate of the carbon skeleton. Besides, the Co leaching was effectively attenuated from 1.86 mg/L(Co@NC) to 0.78 mg/L (Co-Fe@NC-0.2) by the core-shell structure and bimetal strategy. Both O 2 · - and 1 O 2 contributed to the degradation of TBBPS according to quenching experiments. TBBPS was deeply degraded into small-molecule compounds through three degradation pathways by the Co-Fe@NC-0.2/PMS system. This study provides a new strategy for designing highly efficient bimetal–carbon composites for environmental remediation.
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ELECTROCHIMICA ACTA
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2024
·
IF 5.5
Daming Feng,Lixue Zhou,Chang Liu,Hui Li,Yusheng Zhang,Yali Yao,Tianyi Ma
Electrocatalytic nitrogen reduction reaction (NRR) for the synthesis of ammonia (NH 3 ) is one of the green and mild methods of artificial nitrogen fixation, promising as an alternative to replace the existing industrial process. Under the requirements of green chemistry and sustainable development, the design and development of highly active and stable electrocatalysts is very important for improved synthesis performance. Mimicking from the natural nitrogenase, Fe and Mo based catalysts have attracted much attention due to their superior catalytic performance for N 2 adsorption and activation. In this work, an interfacial engineering strategy has been used to prepare a Fe, Mo-bimetallic electrocatalyst for the electrosynthesis of NH 3 . In detail, the pre-pyrolyzed biochar-based Fe 2 O 3 composites were decorated with nano-flowered MoS 2 /MoO 2 hybrids by a solvothermal process (MoS 2 /MoO 2 @Fe 2 O 3 /BC). As confirmed by the extensive characterization, the further modification not only introduced functional counterparts into the electrocatalysts but also regulated the morphology of the nanostructure. The electrochemical tests showed that the highest NH 3 yield rate of MoS 2 /MoO 2 @Fe 2 O 3 /BC was 4.87 μg h − 1 cm −2 and highest FE was 16.5% in 0.1 M Na 2 SO 4 . The catalytic stability and durability were also presented in the longtime electrolysis and cycling experiments. The improved catalytic performance of decorated catalyst, as evidenced by the comparison with Fe 2 O 3 /BC, is attributed to the increased electrocatalytic active area, the moderated hydrophilicity, and the synergistic effect of Fe, Mo-bimetallic active sites. This study provides a new perspective for the design and development of low-cost transition metal complexes as electrocatalysts for nitrogen reduction reactions.
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Journal of Water Process Engineering
·
2024
·
IF 6.3
Fangfang Liu,Mengnan Lu,Xiao Yang,Yuedi Wang,Chunmei Wang,Xiaomin Dou
This work proposed introducing nanoscale Fe-Zr oxides onto the layered-surfaces of MXene carriers to maintain well dispersion and anchoring stabilization. The results indicated that Fe-Zr oxide/MXene has a superior adsorption capacity of 209.1 mg/g at pH 7.0. The mass transfer of antimonite onto Fe-Zr oxide/MXene was investigated by numerical solving the homogeneous surface diffusion model. The external mass transfer coefficient ( k f ) and surface diffusion coefficient ( D S ) were determined to be 6.48 × 10 −4 and 1.86 × 10 −8 cm/min, respectively, and the latter was rate-limited. The 2-D profiles of Sb(III) diffusion within the adsorbents were visualized. Data mining and knowledge discovery using machine learning models indicated that the gradient boosting regression (GBR) model successfully predicted the test datasets. The operational conditions outweigh adsorbent properties in capacity prediction, and equilibrium concentration and adsorbent dose, are the most two important features. Using the trained GBR model, the Sb(III) adsorption capacities of MXene (Ti 3 C 2 ) and Fe-Zr/MXene were well predicted. This work provides insights on understanding the mass transfer mechanisms of Sb(III) in functionalized-MXene adsorbents and employing machine learning models for tuning the treatments for better achievements.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Wenjing Yang,Chuanyin Zhou,Chongxian He,Youwen Yang,Wurikaixi Aiyiti,Liang Xu,Cijun Shuai
The demand for breast mesh with antitumor properties is critical in post-mastectomy breast reconstruction to prevent local tumor recurrence. Molybdenum-based oxide (MoO x ) exhibits enzyme-like activities by catalyzing endogenous hydrogen peroxide to produce reactive oxygen species for inducing tumor cell apoptosis. However, its catalytic activity is limited by insufficient active sites. Herein, a defect engineering strategy is proposed to create redox nanozymes with multiple enzymatic activities by incorporating Fe into MoO x (Fe-MoO v ). Fe-MoO v is subsequently integrated into polycaprolactone (PCL) to fabricate breast meshes for establishing an enzyme-catalyzed antitumor platform. The doping of Fe into MoO x formed numerous defect sites, including oxygen vacancies (OV) and Fe substitution sites, synergistically boosting the binding capacity and catalytic activity of Fe-MoO v . Density functional theory calculations demonstrated that the outstanding peroxidase-like catalytic activity of Fe-MoO v resulted from the synergy between OV and Fe sites. Additionally, OV contributes to the localized surface plasmon resonance effect, enhancing the photothermal capability of the PCL/Fe-MoO v mesh. Upon near-infrared laser exposure, the catalytic activity of the PCL/Fe-MoO v mesh is further improved, leading to increased generation of reactive oxygen species and enhanced antitumor efficacy, achieving 86.7% tumor cell mortality, a 264% enhancement compared to the PCL/MoO x mesh.
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PubMed
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yeshuang Wang,Mingxian Duan,Zhelin Su,Chao Yang,Yuxiao Wang,Tian Kou,Jiawei Kou,Huiling Fan
Cu–1,3,5-benzenetricarboxylate (Cu–BTC) exhibited potential for hydrogen sulfide (H 2 S) removal, however, its sulfur capacity is limited due to it relies only on the adsorption reaction path. Herein, a series of Fe-doped Cu–BTC materials (denoted as x Fe–Cu–BTC) were synthesized to enhance H 2 S removal capacity via a adsorption–oxidation bifunctional synergism mechanism. The prepared materials were characterized using various techniques, and their H 2 S removal performance was measured under dry and ambient conditions. The experimental results demonstrated that the 18%Fe–Cu–BTC shown the optimal breakthrough sulfur capacity of 122.8 mg S/g, marking a 2.1-fold and 10.3-fold improvement over pure Cu–BTC and Fe–BTC, respectively. The characterization analyses revealed that the Cu 2+ active sites initially react with H 2 S to form CuS, while the incorporated Fe 3+ sites trigger the oxidation of CuS, yielding elemental sulfur, Cu 2+ and Fe 2+ . The resultant Cu 2+ and Fe 2+ further engage in reactions with H 2 S to form CuS and FeS, thereby enhancing the H 2 S removal capacity via dual reaction pathways of adsorption and oxidation. Additionally, appropriate Fe doping increased the specific surface area and pore volume of Cu–BTC, which exposed more active sites and improved molecular diffusion. Based on the obtained findings, a plausible desulfurization mechanism involving adsorption and oxidation synergism for remove H 2 S was proposed.
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Catalysis Science & Technology
·
2024
·Vol. 14
·期 3
·667-672
·
IF 4.4
Qiulan Huang,Ruiqin Ren,Jia Li,Muhammad Waqas,Pan Chen,Xiaotian Liu,Dujuan Huang,Zhongyun Yang,Xinglan Peng,Du-Hong Chen,Youjun Fan,Wei Chen
Fabricating highly competent and cost-effective catalysts is essential for promoting the sluggish kinetics associated with the oxygen reduction reaction (ORR). Herein, a new type of Fe, Co decorated porous carbon composite catalyst co-doped with S and N (FeCo–SNC) was prepared by a simple carbonization process. Interestingly, FeCo–SNC inherits not only the pore structure but also the large surface area of the ZIF-67 dodecahedron. Furthermore, the electronic configuration of the two catalytic centers in Fe–N–C and Co–NC was customized. On the basis of synergetic coordination between the two active sites, the fabricated FeCo–SNC showed prior stability for the ORR even after 10 000 cycles of cyclic voltammetry measurement, besides the great limiting current density of 5.99 mA cm−2 and high half potential of 0.856 V (vs. reversible hydrogen electrode), surpassing the commercially available Pt/C catalyst. Moreover, the primary active site of Fe–N–C was regulated, providing the highest catalytic activity for the ORR. This research offers a new perspective on enhancing carbon-based catalysts for the ORR without relying on precious metals and introduces a strategic method for controlling active centers.
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LANGMUIR
·
2024
·
IF 3.7
Ke Zhang,Yafeng Bai,Liying Wang,Yang Gao,Xuesong Li,Xijia Yang,Wei Lü
Zinc-ion hybrid capacitors (ZIHCs) are expected to become the next generation of energy storage devices, highly anticipated for their battery-like performance and lower cost. However, because of their unmanageable structural deformation and inadequate cycling capabilities, they face significant difficulties and challenges in practical production and applications. In this paper, we developed and assembled a flexible solid-state zinc ion hybrid capacitor, which utilizes a gel electrolyte, activated carbon (AC) as the anode, and porous Fe3+ doped MnO2 (Fe-MnO2) as the cathode. The embedding of Fe3+ in MnO2 broadens the original ion channels and provides more electrochemically active sites. The gel electrolyte is formed with poly(vinyl alcohol) (PVA) providing a flexible framework, carboxymethylcellulose (CMC) offering rigid support, and enhanced low-temperature performance due to the addition of ethylene glycol (EG). This combination results in excellent mechanical properties and high ionic conductivity, ensuring stability even under low-temperature conditions. As a result, the flexible ZIHC showcases exceptional specific capacitance, achieving a capacitance of 848.8 mF cm–2 at a current density of 2 mA cm–2, and strong stability when subjected to bending tests. Notably, even under low-temperature conditions of −20 °C, the device maintains consistent electrochemical performance, with a remarkable cycle retention rate of 93.75% after 15 000 cycles. This study demonstrates significant advancements in energy storage systems, creating opportunities for the use of flexible devices across a range of applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Zhu Xiong,Yuhang Cheng,Kaige Dong,Mahmud Sakil,Zhu Wang,Liguo Zhang,Tangfu Xiao,Gaosheng Zhang,Shuaifei Zhao
Super trace thallium(I) (Tl + ) is still highly toxic and its removal from surface water is challenging. Here, we developed a new adsorptive membrane by immobilizing bimetal (cobalt and iron) Prussian blue analogues (Co@Fe-PBAs) on a polytetrafluoroethylene microporous membrane (Co@Fe-PBAs-M). The prepared membrane displayed precise adsorption of trace Tl + (50 μg/L) from complex water. A variety of interfering factors, such as water pH, competitive adsorption of positive ions (Na + and K + ) and negative ions (CO 3 2– and PO 4 3- ), natural organic matters (e.g., fulvic acid and bovine serum albumin) were evaluated during Tl removal. The composite membrane showed high removal efficiency (over 80 %) during long-term dynamic membrane separation of surface water containing super trace Tl + (<2.0 μg/L), breaking through the adsorption limitation in ultralow concentration of Tl + . The unique bimetal electron transfer of Co@Fe-PBAs-M reinforced the adsorptive performance to Tl + through dual ion exchange and intercalation. In the treatment of real Pearl River water containing 0.5 μg/L of Tl + , our membrane effectively reduced the Tl + concentration to 0.04 μg/L during 6-h continuous separation, which was far below the required level for drinking water (i.e., 0.1 μg/L). This work offers a promising solution for safe drinking water by remedying ultralow Tl + contaminated surface water.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Enhao Zhang,Sisi Yao,Xiaoxuan Guo,Xinyi Zhou,Yutai Li,Feifan Xie,Yonghang Wei,Dongjiang Yang,Jin Sun,Yun Lu
The advancement of highly efficient bifunctional electrodes tailored for water electrolysis, specifically targeting the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), is pivotal for sustainable hydrogen production. However, sluggish reaction kinetics and elevated overpotentials pose formidable hurdles. In this study, an innovative strategy is introduced by integrating Fe@ZIF-67 onto self-supporting carbonized rattan stem (CR), leveraging its distinctive through-channel macroporous architecture to bolster catalytic efficacy. The self-supporting CR substrate not only enhances mass transport but also facilitates uniform deposition of ZIF-67, ensuring optimal exposure of active sites. A comparative analysis with carbonized basswood (CW) underscores the superior performance of the macroporous CR substrate in augmenting both OER and HER activities. Notably, the Fe@ZIF-CR self-supported electrode achieves an overpotential of 208 mV at 10 mA cm⁻² for oxygen evolution and 317 mV at 100 mA cm⁻² for hydrogen evolution. Additionally, the self-supporting nature of the CR substrate guarantees long-term stability and mitigates catalyst loss during operation. These findings underscore the synergistic advantages of the macroporous structure and ZIF-67 active sites, offering fresh perspectives on the utilization of biomass-derived carbon materials in sustainable energy technologies.
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Catalysts
·
2024
·Vol. 14
·期 7
·394
·
IF 3.8
Yingjun Ma,Jie Wang,Hangning Liu,Lin Wang,Changhui Sun,Liangyu Gong,Xiaogang Zhang,Jiefang Zhu
Electrochemical water-splitting is widely acknowledged as a renewable strategy for hydrogen production, but it is primarily constrained by the sluggish reaction kinetics of the anode oxygen evolution reaction (OER). In our study, we employ a fast room-temperature corrosion engineering strategy for the construction of a sulfur-doped Ni-Fe layered dihydroxide catalyst (S-NiFe LDH). With the assistance of a sulfur source, microsphere morphology with an ultra-thin lamellar surface cross-arrangement can be rapidly grown on the surface of an iron foam substrate, ensuring a substantial electrochemical interface. The composition of Ni species in the catalysts can be regulated by simply adjusting the amount of Ni2+and reaction time. Functioning as an OER catalyst, the S-NiFe LDH demonstrates high activity and reaction kinetics, featuring a minimal overpotential of 120.0 mV to deliver a current density of 10 mA cm−2, a small Tafel slope of 39.5 mV dec−1and a notable electrical double-layer capacitance (Cdl) of 31.3 mF cm−2. The remarkable electrocatalytic performance can be attributed to its distinctive three-dimensional (3D) structure and sulfur dopants, which effectively regulate the electrochemical interface and electronic structure of NiFe LDH. This work provides valuable insights for expeditious materials design.
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RSC Advances
·
2024
·Vol. 14
·期 33
·24055-24065
·
IF 3.9
Xiuzhen Wei,Zelong Chen,Mengjia He,Liangliang Xu,Yue Li,Jia Yang,Xuekang Zhang,Xianghao Zhang,Ze Wang,Shiyu Cao,Qinghua Zhou,Bingjun Pan
Mg–Fe layered hydroxide (LDH) was synthesized by the double titration method and added to trimesoyl chloride (TMC) to prepare an Mg–Fe LDH-modified polyamide nanofiltration (NF) membrane by interfacial polymerization (IP). Compared to the pure polyamide NF membrane, the Mg–Fe LDH-modified membrane presented a wrinkled structure and a comparatively smooth surface. Additionally, the permeation flux and rejection rate of the modified NF membrane for 1000 mg L−1 Na2SO4 solution were 61.7 L m−2 h−1 and 95.9%, respectively. When the Mg–Fe LDH modified NF membrane was used to separate dye/NaCl mixed solutions, the rejection of NaCl was less than 17% and the rejection rate of Coomassie Brilliant Blue (CBB) molecules was close to 100%. At the same time, the concentration of CBB increased from 500 mg L−1 to 1151 mg L−1 which means that the LDH modified NF membrane could separate CBB/NaCl effectively and could concentrate CBB at the same time.
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