JOURNAL OF APPLIED POLYMER SCIENCE
·
2025
·
IF 2.8
Shangsong Han,Yong Wang,Binhong Gan,Jun Cai,Siyi Jiang,Cuiyu Huang,Shanshan Li
MIL-53(Fe), as a typical metal–organic framework (MOFs) material, has shown broad application prospects in the field of membrane separation technology due to its advantages such as high specific surface area and good chemical stability. However, few studies have specifically applied it to the preparation of oil–water separation membranes. Therefore, this study innovatively proposed a self-assembly strategy. By constructing a MOFs composite coating covering the membrane surface and a comprehensive metal polyphenol network (MPN), this approach was designed to form an efficient, comprehensive oil-rejection system while significantly enhancing pure water flux. Then, through a series of characterizations and performance tests, the results showed that the prepared composite membrane exhibited excellent oil–water separation performance: pure water flux was as high as 3641.21 L m −2 h −1 , and at the same time, the rejection rate of oil-in-water emulsion was stably maintained at more than 99.58%. Therefore, this study not only successfully verified the great potential of MIL-53(Fe)-based composite membranes in the field of efficient oil–water separation, providing a new theoretical basis and feasible technical path for its design, but also further expanded the practical application prospects of MOFs materials in the treatment of oily wastewater, opening up new ideas for the development of the next generation of high-performance separation membranes.
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Nature Energy
·
2021
·Vol. 6
·期 6
·614-623
·
IF 60.858
Gao Ruijie,Wang Jian,Huang Zhen-Feng,Zhang Rongrong,Wang Wei,Pan Lun,Zhang Junfeng,Zhu Weikang,Zhang Xiangwen,Shi Chengxiang,Lim Jongwoo,Zou Ji-Jun
Platinum is the archetypal electrocatalyst for oxygen reduction—a key reaction in fuel cells and zinc–air batteries. Although dispersing platinum as single atoms on a support is a promising way to minimize the amount required, catalytic activity and selectivity are often low due to unfavourable O 2 adsorption. Here we load platinum onto α-Fe 2 O 3 to construct a highly active and stable catalyst with dispersed Pt–Fe pair sites. We propose that the Pt–Fe pair sites have partially occupied orbitals driven by strong electronic coupling, and can cooperatively adsorb O 2 and dissociate the O=O bond, whereas OH* can desorb from the platinum site. In alkaline conditions, the catalyst exhibits onset and half-wave potentials of 1.15 V and 1.05 V (versus the reversible hydrogen electrode), respectively, mass activity of 14.9 A mg −1 Pt (at 0.95 V) and negligible activity decay after 50,000 cycles. It also shows better performance than 20% Pt/C in a zinc–air battery and H 2 –O 2 fuel cell in terms of specific energy density and platinum utilization efficiency.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Yangyang Liu,Fengdi Tu,Ziyu Zhang,Zigang Zhao,Pan Guo,Lixiao Shen,Yunlong Zhang,Lei Zhao,Guangjie Shao,Zhenbo Wang
Iron and nitrogen co-doped carbon (Fe/N/C) electrocatalysts have great potential to catalyze the kinetically slow oxygen reduction reaction (ORR). Unfortunately, the ORR performance of existing Fe/N/C catalysts is seriously hindered by the insufficient density and accessibility of the atomic Fe-N x moieties. Herein, the carboxylate (OAc) molecular scissor is proposed to tailor Fe doped zeolitic-imidazolate-framework-8 (ZIF-8) at atomic scale and construct a multi-dimensional concave Fe@NC catalyst structure (Fe@MNC-OAc). This molecular scissoring strategy imparts Fe@MNC-OAc with dense accessible active sites, multidimensional mass transfer pathways, hierarchical porous structure, and entangled carbon nanotubes network. Therefore, the tailored Fe@MNC-OAc electrocatalyst exhibits excellent ORR activity in acidic media with a half-wave potential of 0.838 V, which is comparable to state-of-the-art non-precious metal catalysts. When assembled as cathode catalyst in a H 2 -O 2 proton exchange membrane fuel cell, it delivers a peak power density of 903 mW cm −2 . This work provides a new approach to tailoring the catalyst architecture and improving the accessibility of active sites.
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Advanced Composites and Hybrid Materials
·
2025
·Vol. 8
·期 6
·394
·
IF 21.8
Wu Chongji,Yang Lu,Qian Zhu,Yan Zupeng,Sun Xia,Hu Weiqiang,Ma Zongqing
The conventional sintered W-Ni-Fe alloy encounters challenges in achieving both high strength and plasticity simultaneously, primarily due to its inadequate organizational compatibility. To address this issue, we developed a novel approach combining in situ freeze-drying and straightforward liquid-phase sintering techniques to effectively control the microstructure of 93W-4.9Ni-2.1Fe alloys. The corresponding W-Ni-Fe alloy in this work simultaneously takes into account ultrafine W grains (28.3 µm), low W-W connectivity (CW-W = 0.31), and suitable γ phase volume fraction (20.2%), which is currently difficult for traditional W-Ni-Fe alloys to achieve. The minute dimensions of nanopowder play a crucial role in inhibiting Ostwald ripening and facilitating W grain refinement. Additionally, the extensive surface area of nanopowder enhances capillary penetration, leading to effective homogenization of high γ phase volume. As a result, the freeze-dried W-Ni-Fe alloy simultaneously achieves high strength (1010 MPa) and high plasticity (31%), which provides a new insight for the further development of W-Ni-Fe alloy industries.
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Shu-Hu Yin,Xiao-Yang Cheng,Yu Han,Ting Zhu,Zhong-Wei Yu,Rui Huang,Jun Xu,Yan-Xia Jiang,Shi-Gang Sun
Fe-N-C catalysts are promising substitutes for precious-metal platinum in acidic oxygen reduction reactions (ORR), yet their moderate intrinsic activity and susceptibility to reactive oxygen species (ROS)-induced degradation hinder practical implementation. Herein, we fabricate a Ru-Fe dual-site catalyst (RuFe-N-C) through a two-step pyrolysis strategy. Structural characterization reveals atomic-scale proximity between Ru single atoms and Fe-N 4 moieties, exhibiting a projected distance of ~1.7 Å. This configuration induces Fe–N bond elongation accompanied by 2.5% lattice distortion. The optimized RuFe-N-C catalyst exhibits high ORR performance, with a half-wave potential ( E 1/2 ) of 0.840 V and peak power density ( P max ) of 938 mW cm –2 under 150 kPa absolute H 2 -O 2 . These metrics signify substantial enhancements relative to conventional Fe-N-C benchmarks (+21 mV in E 1/2 and +42% in P max ). Moreover, the catalyst maintains outstanding stability, showing merely 17 mV E 1/2 decay after 10000 accelerated durability test (ADT) cycles. Experimental analyses reveal a bifunctional mechanism: (1) Adjacent Ru sites substantially enhance the intrinsic ORR activity of Fe-N 4 moieties, delivering a notable turnover frequency (TOF = 17.86 e site –1 s –1 at 0.85 V vs. RHE) that exceeds state-of-the-art Fe-N-C benchmarks by 1–2 orders of magnitude (< 1 e site –1 s –1 ); (2) Ru centers function as electron relays that facilitate ROS scavenging, thus suppressing degradation. This work establishes a paradigm for engineering bimetallic single-atom catalysts through synergistic electronic modulation to concurrently enhance activity and stability.
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Matter
·
2024
·
IF 17.3
Lingfeng Li,Jiaming Zhu,Fanpeng Kong,Yijie Wang,Cong Kang,Ming Xu,Chunyu Du,Geping Yin
Elucidating how the local strain environment of single atoms affects their impact on a sluggish acidic oxygen reduction reaction (ORR) is important for the design and construction of highly active electrocatalysts. Here, we report that the atomic strain geometry of Fe single sites is exclusively regulated by the communicative effects of dual atoms. Theoretical analysis reveals that Fe-Ru dual atoms in a moderate strain environment achieve the lowest Gibbs free energy barrier during an ORR. Impressively, FeRu-N-C with an FeRuN 8 moiety exhibits the highest acidic ORR performance, with a half-wave potential ( E 1/2 ) of 0.860 V and only a 17-mV loss in E 1/2 after 50,000 potential cycles. Operando characterization and electronic configuration analysis demonstrate that moderately strained Fe sites promote hydrogenation desorption of (oxy-)hydroxyl by enabling more electrons to occupy antibonding orbitals. This study describes a promising way of investigating high-performance single-atom-based catalysts by tailoring the atomic strain environment.
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WATER RESEARCH
·
2024
·
IF 11.4
Kexin Yin,Xing Xu,Qinyan Yue,Yanan Shang,Yanwei Li,Yue Gao,Baoyu Gao
The limited interaction between pollutants, oxidants, and the surface catalytic sites of single atom catalysts (SACs) restricts the water decontamination effectiveness. Confining catalytic sites within porous structures enables the localized enrichment of reactants for optimized reaction kinetics, while the specific regulatory mechanisms remain unclear. Herein, SACs with porous modification significantly improves the utilization of peroxymonosulfate (PMS) and pollutant degradation activity. Confining catalytic sites in porous structure effectively reduces the mass transfer distance between radicals (SO 4 •- and •OH) and pollutants, thereby improving reaction performance. Pore modulation changes the surface electronic structure, leading to a significant improvement in the electron migration process. The system shows significant potential in effectively oxidizing various common emerging pollutants, and exhibits robust resistance to interference from environmental matrices. Moreover, a quantitative evaluation using life cycle assessment (LCA) indicates that the pFe-SAC/PMS system showcases superior environmental importance and practicality.
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ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Haozheng Hu,Xianghao Meng,Yin Li,Yusong Yang,Yanqiu Xu,Junxian Hu,Yaochun Yao
In the era of extensive deployment of LiFePO4 batteries in energy storage and electric vehicle domains, the recycling of lithium from spent LiFePO4 (SLFP) batteries has emerged as a focus, which helps in alleviating environmental pollution and resource shortages. Traditional recycling techniques, encompassing pyrometallurgical and hydrometallurgical methods, are often marred by low selectivity and extraction efficiency. Herein, an eco-friendly and low-consumption recycling strategy involving potassium pyrosulfate (K2S2O7)-assisted low-temperature roasting and subsequent water leaching has been developed for selectively recycling Fe and Li from SLFP batteries. The proposed strategy, compared to the conventional inorganic acid leaching method, mitigates the environmental hazards caused by acidic wastewater generation and reduces the costs associated with wastewater treatment. Investigations of thermal performance characterization and thermodynamic calculation analyses have revealed that K2S2O7 plays a pivotal role in extracting lithium from the Fe–P–O framework, converting lithium into a soluble sulfate variant and iron into insoluble compounds. This process culminates in the segregation of a lithium-rich leachate and an iron-enriched residue, which are further processed to synthesize Li2CO3 and FePO4. The effects on Li leaching of the mass ratio of K2S2O7 to SLFP, roasting time, roasting temperature, and water leaching time are systematically studied and 95.87% Li was leached in water under optimal conditions. In addition, the feasibility of the strategy was further illustrated by the regeneration of LiFePO4 produced by the recycled Li2CO3 and FePO4. Overall, this recovery strategy stands out for its effective lithium-iron segregation, environmental sustainability, and economic viability, which provide some inspiration for high-efficiency and environmentally friendly recovery metal from spent lithium-ion batteries.
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MICROCHIMICA ACTA
·
2025
·Vol. 192
·期 3
·1-10
·
IF 5.3
Han Hongyu,Huang Yiqun,Miao Junjian,Lai Keqiang
Surface-enhanced Raman spectroscopy (SERS) was combined with stoichiometric analysis to synthesize a AuNPs@MIL-100 (Fe) SERS substrate. This high-performance, and low-cost metal–organic framework-based SERS nano sensor is capable of detecting malachite green (MG) residues in fish. The minimum detectable concentration of MG in standard solutions is 0.1 μg/L, while in fish samples, the detection range spanned from 0.003–0.088 μg/kg. The partial least squares regression (PLSR) and support vector machine regression (SVR) were applied to model the SERS data, enhancing both the precision and reliability of the detection. The results show that compared with the traditional linear regression and PLSR models, the prediction accuracy of the SVR model is an improvement with higher stability. MG standard solutions and three fish samples can be analysed directly or after simple extraction. This method can be used to detect trace harmful substances in different aquatic products. Graphical
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MINERALS ENGINEERING
·
2024
·
IF 4.9
Qinbo Cao,Yan Yan,Heng Zou,Haiyu Zhang,Dianwen Liu,Shuming Wen,Yanjun Li
The separation of galena (PbS) from chalcopyrite (CuFeS 2 ) requires strong oxidants for the depression of PbS, due to the excellent hydrophobicity of PbS. In this work, an advanced oxidation process, i.e., S 2 O 8 2− /Fe 2+ treatment, was employed to selectively depress PbS. The parameters of the S 2 O 8 2− /Fe 2+ process were determined via flotation tests as follows: pH 3, 1:1 S 2 O 8 2− : Fe 2+ molar ratio, and 10 min reaction time. The S 2 O 8 2− /Fe 2+ treatment selectivity decreased the hydrophobicity of the PbS surface. UV–vis spectroscopy results revealed that SO 4 − (major species) and OH radicals were produced in solution by the activation of Fe 2+ . The SO 4 − / OH radicals reacted with the PbS surface, generating the SO 4 2− and PbSO 4 species. These species coated the PbS surface, forming a hydrophilic PbS surface and inhibiting the PbS flotation. By contrast, the S 2 O 8 2− /Fe 2+ treatment generated only a minimal amount of SO 4 2− (5.98 % of the total S species) on the CuFeS 2 surface. Therefore, the CuFeS 2 surface was hydrophobic and CuFeS 2 particles could still be floated into the foam phase. This study provides a promising method for the selective depression of PbS in the PbS-CuFeS 2 mixture.
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RSC Advances
·
2024
·Vol. 14
·期 24
·16747-16757
·
IF 3.9
Siyi Mi,Lungang Chen,Xinghua Zhang,Qi Zhang,Longlong Ma,Jianguo Liu
One of the main obstacles to the development of sustainable biomass feedstocks today is the research of selective hydrogenation of biomass platform compounds for the synthesis of high-value chemicals. This work reports on the synthesis of a Ni/Fe bimetallic catalyst with nitrogen-doped carbon serving as the carrier, hydrogen serving as the primary donor, and isopropanol serving as the reaction medium and serving as a secondary donor. Vanillin was catalytically hydrogenated to produce 4-methylguaiacol, a complete hydrogenation product, under a reaction temperature of 200 °C for four hours. A single product with a good yield (95.26% conversion and selectivity up to 99%) was achieved by the moderate conditions, offering a potential route for the catalytic hydrogenation of biomass platform compounds.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Chen Yuanxing,Qin Ying,Liu Mingwang,Yang Wenhong,Qiu Yiwei,Li Wen,Zheng Lirong,Gu Wenling,Zhu Chengzhou,Hu Liuyong
Energy level mismatches between semiconductors and cocatalysts often induce carrier recombination, limiting photocatalytic and photoelectrochemical (PEC) efficiency. Here, we integrate Pt nanocluster-Fe single-atom pairs with CuO to regulate both solid-solid and solid-liquid interfaces in PEC systems. Experimental and theoretical analyses reveal that an Ohmic contact at the CuO/Pt interface accelerates electron extraction, while Pt-to-Fe charge transfer enhances oxygen reduction at Fe sites, collectively boosting reaction kinetics. Leveraging this, we construct a PEC biosensor exploiting chelating effect of glyphosate on CuO to impede electron transfer, achieving a detection limit of 0.41 ng/mL. This interface engineering strategy advances cocatalyst design for enhanced energy conversion and sensing applications by simultaneously addressing carrier dynamics and interfacial reaction barriers.
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