Catalysis Science & Technology
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2025
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IF 4.2
ChengBo Qian,Yuyuan Yao,Hongliang Zhu
Fe-based catalysts have garnered significant attention due to their high stability, low toxicity and cost-effectiveness, while the construction of highly active heterogeneous Fe-based catalysts through a simple method is still challenging in the environmental catalysis field. Herein, employing the synergistic enhancement effect of the conductive polymer polyaniline (PANI) and co-catalyst MoS2, a highly active PANI-supported Fe-doped MoS2 catalyst (PANI-Fe@MoS2) was prepared via a facile one-step hydrothermal process. Surprisingly, PANI incorporation induced critical structural modifications, including reduced average particle size (1 μm), expanded interlayer spacing (1.09 nm), and enhanced sulfur vacancy density. Interestingly, PANI-Fe@MoS2 achieved nearly 100% elimination of carbamazepine (CBZ) within 10 min, and its removal efficiency (k-value) surpassed most of those reported in the literature. Notably, PANI-Fe@MoS2 exhibited a high removal of TOC (nearly 50%), a wide pH operating range (2–10), and outstanding removal efficiency for various contaminants. Additionally, the quenching and electron paramagnetic resonance (EPR) experiments revealed that singlet oxygen (1O2) and hydroxyl radicals (˙OH) were the main reactive oxygen species (ROSs) for degrading CBZ. Moreover, the potential degradation pathways were proposed based on the intermediates of CBZ. This work provides a strategic paradigm for designing efficient heterogeneous Fe-based catalysts for environmental remediation.
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Journal of Materials Chemistry A
·
2025
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IF 9.5
Qin Tang,Lingyue Wang,Shenglong Zhang,Pengfei Xue,Yuye Zhang,Hongbo Li,Dongdong Zhu
It is critical to develop highly efficient electrocatalysts for water splitting to achieve energy-saving hydrogen production. Recently, fullerene-based electrocatalysts have been widely reported for cathodic hydrogen evolution reaction (HER), while their application for intrinsically sluggish oxygen evolution reaction (OER) at the anode has been rarely explored. Herein, a novel OER electrocatalyst, NiFe-OC60, was prepared by introducing Ni and Fe species on fullerol C60(OH)x. Fullerene-based carbon support can provide a high surface area, and be served as an electron buffer due to its inherent electron-withdrawing property. Besides the synergistic effects between Ni and Fe, fullerene-based carbon support promotes the generation of high-valence Ni3+ species, thus contributing to improved OER performance. The as-synthesized NiFe-OC60 supported on glassy carbon electrode exhibits excellent OER results with a relatively small overpotential of 314 mV at the current density of 10 mA cm−2, and a small Tafel slope of 38.62 mV dec−1 in the alkaline solution. Our work demonstrates fullerene-based materials as promising electrocatalysts for emerging clean-energy related technologies.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Junhao Cui,Zhiyang Zhao,Yongqi Ren,Bailong Chen,Chase Rheinlander,Antonio Xavier Moore,Longzhi Li
Microwave-assisted hydrogenolysis of lignin is an emerging alternative to conventional depolymerization capable of converting lignin into aromatic compounds. Activated carbon (AC) supported Fe component have been shown to be cost-effective for this process, but its cycle stability needs to be improved due to Fe agglomeration. Herein, a strategy of nitrogen doping to promote stability was developed, which utilized melamine (C 3 H 6 N 6 ) as nitrogen source to prepare the catalyst of N-doped AC supported Fe (Fe/N-AC). The catalyst characterization indicated that the N-doped AC acted as anchor points for Fe components, avoiding catalyst deactivation from the source. Fe/N-AC presented an excellent cycle stability, remaining a phenolic compound selectivity of 93.3 % after five cycles and a decrease of only 4.79 % (compared to the first). The DFT calculation results revealed that Fe/N-AC tended to break C Ar -OCH 3 during the hydrogenolysis of guaiacol, with an energy barrier of 0.877 eV. This work proposes a simple and effective strategy to improve the stability of lignin hydrogenolysis catalysts, providing important references for the high-valued utilization of lignin.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Yujia Tong,Chenxuan Shao,Jinbo Chen,Fiona Hammond Quarcoo,Changqing Miao,Xiaohui Ju,Weixing Li
High hydrophobicity of polyvinylidene fluoride (PVDF) membrane surface results in adsorption of oil droplets and membrane fouling . A hydrogel coating with crosslinking network of polyvinyl alcohol (PVA), pyrogallol (PG) and Fe(III) based on PVDF membrane was proposed. Hydrogen bonds between PVA and PG in water were regulated by ethanol to form a uniform hydrophilic hydrogel coating on PVDF membrane. Chelation between PG and Fe 3+ significantly enhanced hydrogel adhesion. The surface energy of the developed PVDF-PVA/PG-Fe 3+ membrane was 39.96 mJ·m −2 , 2.71 times that of the pristine PVDF membrane, while its adhesion to oil is close to 0 μN. The permeate flux reached 1341 L·m −2 · h −1 at 0.1 bar for separating isooctane-in-water emulsions with good separation efficiency (>99 %) and cycling stability. The developed membrane could also effectively separate petroleum ether-in-water and dodecane-in-water emulsions.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Yang Wang,Meili Ding,Wei Rong,Suyu Kong,Jianfeng Yao
Photodriven CO 2 conversion has been widely recognized as an effective pathway for achieving carbon neutrality. In this paper, we demonstrate the immobilization of bimetallic Zn/Fe ZIF onto the surface of Ti 3 C 2 T x MXene via an in situ growth process for photodriven solvent-free CO 2 cycloaddition. MXene can extend the optical response of bimetallic ZIF into the near-infrared region. In turn, the incorporated MOF particles effectively prevent the layers of MXene from stacking. The resulting Zn 20 Fe 1 -ZIF/MXene has improved activity (96% yield) in the cycloaddition of epichlorohydrin with 1 bar CO 2 under full spectrum illumination (350 mW/cm 2 ) for 6 h, ca. 3.4, 1.7, and 1.2 times higher than those of pure Zn 20 Fe 1 -ZIF, MXene, and the physical mixture, respectively. Besides, this hybrid catalyst provides desirable stability and performance even after several catalytic cycles, exposure to humid environment or under diluted CO 2 (15%). Control experiments and infrared thermography reveal the synergistic photocatalytic-photothermal contribution of hybrid materials to the photoinduced CO 2 fixation. Our research offers a facile method to construct MOF containing photocatalysts for application of CO 2 conversion with high practical utility.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Huijie Ni,Shaojie Xu,Rong Lin,Yi Ding,Jinjie Qian
There is significant anticipation for high-efficiency and cost-effective non-precious metal-based catalysts to advance the industrial application of the anodic oxygen evolution reaction (OER) for hydrogen production. This study introduces an efficient strategy that utilizes ligand-induced metal–organic framework (MOF) building blocks for the synthesis of hollow binary zeolitic imidazolate frameworks 67 (ZIF-67) and Prussian blue analogues (PBAs) (ZIF-67@PBA) heterostructures through a hybrid MOF-on-MOF approach. Manipulating the Co 2+ /Zn 2+ ratio in the precursor ZIF-67 allows for the convenient synthesis of the final product, denoted as Co x Fe-ZP, after pyrolysis , where the inclusion of Zn effectively modulates the distribution of Co in the catalyst. The resulting Co x Fe-ZP catalysts exhibit a positive synergistic effect between hollow graphitic carbon nanomaterials and Fe-doped Co nanoparticles. The optimal Co 0.3 Fe-ZP catalyst demonstrates satisfactory OER performance, achieving an overpotential of 302 mV at 10 mA cm −2 and a small Tafel slope of 60.0 mV dec −1 . Further analysis of the activation energy confirms that the enhanced OER activity of Co 0.3 Fe-ZP can be reasonably attributed to the combined influence of its morphology and composition. This study demonstrates a ligand-induced method for examining the morphology and electrochemical properties of grown binary MOF-on-MOF heterostructures for OER applications.
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Journal of Energy Chemistry
·
2025
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IF 14.9
Jing Gao,Qitao Liu,Haotian Wang,Muhammad Bilal Akbar,Zhihua Wu,Jiabo Le,Jianming Li,Qinglu Liu,Yongbo Kuang
CuBi 2 O 4 (CBO) photocathodes hold significant promise for efficient photoelectrochemical (PEC) water splitting due to their favorable band gap and theoretical onset potential. However, their practical application is hindered by poor charge separation efficiency. Herein, we introduce a characteristic in-situ solution Fe-doping strategy that markedly improves photoelectrochemical performance of CBO, doubling the photocurrent density and achieving an unprecedented 190 mV anodic shift in the onset potential. By integrating with an electrochemical oxidation post-treatment, a record incident photon-to-current efficiency (IPCE) exceeding 40% at 0.6 V vs. RHE under visible light illumination is achieved. The versatility of the doping strategy is demonstrated across CBO photocathodes synthesized by different methods with various morphologies, grain sizes, and crystallinities. Mechanistic studies reveal that the gradient distribution of Fe 3+ ions generates an internal electric field that facilitates efficient charge separation and increases acceptor density. The strong Fe–O bonding also enhances structural stability against photo-induced corrosion. Notably, our investigation uncovers the non-temperature-dependent nature of CBO photocurrent, indicating that PEC performance enhancement primarily depends on reducing carrier recombination rather than improving bulk conductivity. This work lays the groundwork for future advancements in water splitting performance of CBO photocathodes, offering a complementary strategy to conventional methods for enhancing charge separation efficiency.
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Journal of Water Process Engineering
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2024
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IF 6.3
Linke Jiang,Ruiqi Wang,Shuiqin Shi,Junmei Yan,Mingbao Feng,Lianbao Chi
With the aging of the global population and continued economic development, the use of sartan-type antihypertensive drugs (e.g., losartan (LOS), telmisartan (TEL), and valsartan (VAL)) has increased with widespread contamination issues. However, the effect of advanced oxidation processes (AOPs) on the degradation of sartans remains unknown. Therefore, AOPs such as the Fe(II)/peroxymonosulfate (PMS) system and ozonation were used to treat the typical sartans, which led to the formation of various transformation products (TPs). This research involves the formation mechanisms of these TPs following AOPs including aldolization, hydroxylation, ring cleavage, carbonylation and cyclization. The risk evaluation focused on the biodegradability and toxicity of the drugs and their TPs, assessed using computerized toxicity prediction software. The findings indicated that the biodegradability of most TPs was generally poor and most TPs exhibited acute/chronic toxicity. This underscores the need for caution when applying AOPs in water treatment to prevent secondary contamination and suggests the potential necessity of integrating AOPs with complementary purification technologies. This research provides novel insights into the degradation pathways and environmental risks of sartans, emphasizing the importance of a holistic approach to water treatment.
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JOURNAL OF THERMAL SPRAY TECHNOLOGY
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2025
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IF 3.3
Zhang Jian,Chen Hongxuan,Pang Xiaotong,Liu Shilong,Misra R. D. K.,Sun Junhao
Currently, surface coatings on agricultural machinery are crucial for extending service life. However, achieving coating strength and toughness remains a challenge. In this paper, two types of high-hardness iron-based coatings, referred as S1 and S2, were prepared by modulating the Mo/V ratio in the Fe-C-V-Mo-B system, and their microstructural evolution and property changes were investigated. The results show that the S1 coating primarily consist of martensitic matrix, spherical VC, blocky Mo 2 B, and a small amount of skeleton-like Mo 2 B. In contrast, the S2 coating consist of martensitic matrix, petal-like VC, and skeleton-like Mo 2 B. Compared with S1, the VC volume fraction in S2 increases by 6.5%, and the Mo 2 B volume fraction increases by 16.3%. The average microhardness of S1 and S2 coatings are 737 HV 0.5 and 954 HV 0.5 , respectively, indicating that the S2 coating exhibits a 22.7% higher microhardness compared with S1. The average friction coefficients of S1 and S2 coatings are 0.434 and 0.398, respectively. Furthermore, the wear loss of S2 coating is approximately half that of S1. The fracture toughness of S1 and S2 coatings are 51.9 MPa·m 1/2 and 51.7MPa·m 1/2 , respectively. Fracture analysis reveals that the skeleton-like eutectic structure in S2 can deflect cracks generated by impact, increase the length of propagation path, and improve the toughness of coating. It allows S2 coating to achieve high hardness and wear resistance, while maintaining toughness comparable to S1 coating. This study provides a theoretical basis for the design and development of iron-based coatings with high hardness, high abrasion resistance, and impact resistance for agricultural machinery.
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CHINESE JOURNAL OF CATALYSIS
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2024
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IF 15.7
Ziyuan Xiu,Wei Mu,Xin Zhou,Xiaojun Han
The electrocatalytic N 2 reduction reaction (NRR) is expected to supersede the traditional Haber-Bosch technology for NH 3 production under ambient conditions. The activity and selectivity of electrochemical NRR are restricted to a strong polarized electric field induced by the catalyst, correct electron transfer direction, and electron tunneling distance between bare electrode and active sites. By coupling the chemical vapor deposition method with the poly(methyl methacylate)-transfer method, an ultrathin sandwich catalyst, i.e., Fe atoms (polarized electric field layer) sandwiched between ultrathin (within electron tunneling distance) BN (catalyst layer) and graphene film (conducting layer), is fabricated for electrocatalytic NRR. The sandwich catalyst not only controls the transfer of electrons to the BN surface in the correct direction under applied voltage but also suppresses hydrogen evolution reaction by constructing a neutral polarization electric field without metal exposure. The sandwich electrocatalyst NRR system achieve NH 3 yield of 8.9 μg h −1 cm −2 and Faradaic Efficiency of 21.7%. The N 2 adsorption, activation, and polarization electric field changes of three sandwich catalysts (BN-Fe-G, BN-Fe-BN, and G-Fe-G) during the electrocatalytic NRR are investigated by experiments and density functional theory simulations. Driven by applied voltage, the neutral polarized electric field induced by BN-Fe-G leads to the high activity of electrocatalytic NRR.
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Journal of Physical Chemistry C
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2024
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IF 3.3
Mingjun Xu,Zhao Jin,Meiling Xiao,Changpeng Liu,Wei Xing
Pyrolyzed iron and nitrogen codoped carbon materials (Fe–N–C) with atomically dispersed Fe-Nx sites have received extensive attention as a highly promising alternative to Pt for oxygen reduction reaction (ORR), yet there remains a considerable performance gap between them. To further improve the catalytic performance of Fe–N–C catalysts, we herein developed a microwave-assisted method to improve both the active site density (SD) and intrinsic activity, thus achieving outstanding ORR activity. The in situ generated Fe precipitation is beneficial to improve the doping efficiency of Fe and the subsequent formation of synergetic active sites, leading to increased SD. Both the X-ray absorption spectroscopy and operando Raman confirmed the copresence of atomic Fe moieties and nanoclusters, in which the nanoclusters synergically promote the activity of the single atomic sites. The enriched synergetic active sites endow the as-prepared catalyst with excellent performance by showing a current density of 42 mA cm–2 at 0.9 V in a proton exchange membrane fuel cell, approaching the DOE 2025 target. This work not only affords a highly active ORR catalyst but also provides a simple and potentially scale-up approach to Fe–N–C catalysts.
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Heliyon
·
2024
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IF 3.4
Yige Yan,Mohan Huang,Yongsheng Wang,Dawei He,Jiaqi He
Metal-organic frameworks (MOF) have been wildly synthesised and studied as electrode materials for supercapacitors, and bimetallic MOF of Ni and Co has been broadly studied to enhance both specific capacitance and stability of supercapacitors. Herein, a best performance (about 320 F/g) of Ni–Co bimetallic MOF was found in a uniform preparation condition by adjusting the ratio of Ni to Co. Then tiny third metal ion was introduced, and we found that the morphology of material has a significant change on the original basis. Furthermore, certain ions (Zn, Fe, Mn) introduced make a huge improvement in capacitance based on Ni–Co MOF of 320 F/g. The result shows that Zn–Ni–Co MOF, Fe–Ni–Co MOF and Mn–Ni–Co MOF perform specific capacitance of 1135 F/g, 870 F/g and 760F/g at 1 A/g, respectively. Meanwhile, the asymmetric supercapacitor (ASC) was constructed by Zn–Ni–Co MOF as positive electrode and active carbon (AC) as negative electrode. The Zn–Ni–Co MOF//AC ASC possesses a energy density of 58 Wh/kg at a power density of 775 W/kg. This research provides a new methods to regulate the morphology of MOF and a novel viewpoint for assembling high-performance, low-price, and eco-friendly green energy storage devices.
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