PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2021
·Vol. 118
·期 21
·e2105610118
·
IF 11.205
Yu Ma,Ding Chen,Zhi Fang,Yapeng Zheng,Weijun Li,Shang Xu,Xianlu Lu,Gang Shao,Qiao Liu,Weiyou Yang
In terms of ideal future energy storage systems, besides the always-pursued energy/power characteristics, long-term stability is crucial for their practical application. Here, we report a facile and sustainable strategy for the scalable fabrication of carbon aerogels with three-dimensional interconnected nanofiber networks and rationally designed hierarchical porous structures, which are based on the carbonization of bacterial cellulose assisted by the soft template of Zn-1,3,5-benzenetricarboxylic acid. As binder-free electrodes, they deliver a fundamentally enhanced specific capacitance of 352 F ⋅ g–1 at 1 A ⋅ g–1 in a wide potential window (1.2 V, 6 M KOH) in comparison with those of bacterial cellulose–derived carbons (178 F ⋅ g–1) and most activated carbons (usually lower than 250 F ⋅ g–1). The as-assembled supercapacitors exhibit an ultrahigh capacitance of 297 F ⋅ g−1 at 1 A ⋅ g−1, remarkable energy density (14.83 Wh ⋅ kg−1 at 0.60 kW ⋅ kg−1), and extremely high stability, with 100% capacitance retention for up to 65,000 cycles at 6 A ⋅ g−1, representing their superior energy storage performance when compared with that of state-of-the-art supercapacitors of commercial activated carbons and biomass-derived analogs.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xue Zhao,Liangfei Duan,Mengshan Chen,Peizhi Yang,Qian Liu,Yuelong Liu,Haoran Zhang,Zhuang He,Guangzhi Hu,Yingtang Zhou
Advanced-oxidation-process (AOPs) based on peroxymonosulfate (PMS) can provide strong reactive oxygen species (ROS) for the elimination of persistent-organic-pollutants (POPs), but the input of highly active environmentally friendly catalysts is the key. Here, confined cobalt was in-situ deposited on natural mineral halloysite nanotubes by Coulomb interaction, which further realizes the introduction of atomically-dispersed cobalt sites in nitrogen-doped hollow-carbon-nanotubes with large specific surface area. The constructed CoNC/NHCNTs-900 material can effectively activate PMS, resulting in the removal rate of tetracycline probe pollutants close to 100%, and the mineralization rate reached a record of 89.07%. Combined with density functional theory calculations, it was proved that the enrichment of graphite nitrogen is beneficial to regulate the microenvironment of Co and promote the adsorption and activation of PMS. In-depth tracking of the formation of ROS and the mechanism of tetracycline mineralization proved that CoNC/NHCNTs-900-driven AOPs degradation of POPs into a low-toxic species has reliability and practical significance.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Minglong Guo,Xiaoyan He,Guangxing Yang,Hongjuan Wang,Feng Peng,Guoqiang Cao,Qiao Zhang,Zhiting Liu
In the realm of CO 2 electrochemical reduction, Bi 2 O 2 CO 3 nanosheets have garnered attention for their ability to selectively produce formate. However, as CO 2 electroreduction technologies advance toward industrial applications, a scalable and green synthesis method is urgently needed. Our research leverages three common Bi-based inorganic salts-BiCl 3 , Bi 2 (SO 4 ) 3 , and Bi(NO 3 ) 3 -as precursors to develop a straightforward process of hydrolysis followed by anions exchange. This method produces high yields of Bi 2 O 2 CO 3 nanosheets without the need for organic solvents or external heating, even at a large scale of ~100 grams, ensuring both sustainability and cost-efficiency. The resulting nanosheets achieved Faradaic efficiencies exceeding 90% across a wide range of potentials for formate production. The combination of innovative synthesis and effective CO 2 conversion underscores the potential of Bi 2 O 2 CO 3 for industrial-scale applications in sustainable energy and chemical production.
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Polymers
·
2026
·Vol. 18
·期 6
·772
·
IF 5.8
Qianyi Wang,Guohan Wang,Sasa Ma,Zichen Wang,Lijie Luo,Yongjun Chen
The widespread use of plastics has inevitably led to the accumulation of persistent plastic debris in aquatic systems, where gradual fragmentation generates microplastics (MPs) that threaten ecological and biological health. Their small size, chemical stability, and resistance to degradation make effective removal particularly challenging. In this work, a composite adsorbent was fabricated through the in situ solvothermal growth of Materials of Institute Lavoisier 100 (Iron) (MIL-100(Fe)) onto coconut shell-derived activated carbon (CSAC), yielding a monolithic material denoted as CSAC@MIL-100(Fe). The integration of porous C with a metal–organic framework created a hierarchically structured adsorbent rich in accessible binding sites. The composite achieved a maximum polystyrene (PS) removal efficiency of 97.4% and maintained 91.44% efficiency after seven regeneration cycles. Stable adsorption performance was observed across a broad pH range. Structural and chemical analyses (scanning electron microscopy (SEM), Brunauer–Emmett–Teller (BET), X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS)) combined with adsorption modeling revealed heterogeneous multilayer adsorption behavior consistent with the Freundlich isotherm and pseudo-second-order kinetics. π–π interactions, electrostatic attraction, and coordination effects jointly governed PS capture. The Langmuir maximum adsorption capacity reached 746.27 mg/g. These findings demonstrate a practical and recyclable strategy for efficient MP remediation in aquatic environments.
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WATER AIR AND SOIL POLLUTION
·
2026
·Vol. 237
·期 12
·702
·
IF 3.5
Yin Shiyu,Du Haiying,Yang Hong,Lai Chunrong
The treatment of industrial wastewater containing multiple heavy metals (MHMs) remains challenging, primarily because conventional adsorbents suffer from poor stability, limited adsorption capacity in mixed-metal systems, or high energy consumption during synthesis. To address these issues, this study employed a room-temperature in-situ impregnation method to load NH 2 -MIL-100(Fe) onto amine-functionalized magnetic hydrochar (HBAP). Three highly dispersible magnetic composites, designated as NM-100-HBAP-X (X = 0.75, 1, 1.25), were synthesized by adjusting the mass ratio of NH 2 -MIL-100(Fe) to HBAP. Experimental results demonstrated that the optimal material (NM-100-HBAP-1) exhibited high adsorption capacities for Pb(II), Cd(II), and Cr(VI) in a mixed-metal system. The maximum adsorption capacities determined by the Langmuir model were 181.13, 175.02, and 158.69 mg/g for Pb(II), Cd(II), and Cr(VI), respectively, which are comparable to previously reported values for hydrochars or MOF-based materials. Mechanistic analysis revealed that amino groups facilitate a synergistic process by reducing Cr(VI) to Cr(III), which is then immobilized via complexation and co-precipitation, thereby further enhancing Cd(II) removal. The material also demonstrated good cycling stability, retaining over 50% of its initial adsorption capacity after five regeneration cycles, and maintained effective performance in various real water samples. Furthermore, toxicity tests confirmed its environmental safety, and life cycle assessment quantified the GWP of producing 1 kg of NM-100-HBAP-1 as 41.224 kg CO 2 eq, with electricity and NH 2 -H 2 BDC synthesis as the dominant contributors. This study not only provides an efficient adsorbent for heavy metal removal but also offers a systematic research framework integrating material design, mechanistic investigation, and environmental assessment for pollution remediation.
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Scientific Reports
·
2026
·Vol. 16
·期 1
·7837
·
IF 4.9
Abou-Elyazed Ahmed S.,Genena Eman E.,El-Sayed Ibrahim E. T.,Abdel-Bary Hamed M.,Tony Maha A.
The photocatalytic Fenton oxidation reaction of paracetamol (PCT), as a widely used pharmaceutical and persistent water contaminant, was investigated using RTG-MIL-100(Fe) framework, prepared via a KI-assisted, solvent free, room temperature synthesis, in the presence of H₂O₂ under UV irradiation. The mild conditions synthesis of RTG-MIL-100(Fe) is investigated, and the material is comprehensively assessed through characterized using X-ray Diffraction (XRD), Scanning Electron Microscopy (SEM), Brunauer–Emmett–Teller (BET), and X-ray Photoelectron Spectroscopy (XPS). The catalytic system is introduced as a source of photo-Fenton-like reaction and demonstrated a dual mechanistic pathway involving both semiconductor-like photoexcitation and open metal site (OMS) activation. The operating Fenton parameters are optimized and the experimental research revealed that the reaction is working at the room temperature using 400 ppm H₂O₂, 20 mg/L of RTG-MIL-100(Fe)at natural pH of wastewater (5.5) and the PCT reached almost complete removal 99.6%. The synergistic interaction of photogenerated charge carriers and OMS-driven Fenton-like processes resulted in efficient oxidative mineralization of PCT to CO₂ and H₂O. Furthermore, the reaction is endothermic in nature and following the first order reaction kinetics. These findings highlight the potential of KI-modified MOF-based photo-Fenton catalysts as sustainable and robust materials for the treatment of pharmaceutical wastewater.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 2
·122011
·
IF 7.5
Di Jin,Yunpeng Zou,Yang Zhao,Shuai Chen,Shiwei Luo,Taotao Chen,Jinchuan Zhang,Jialin Chen,Jijie Li,Yuewen Mu,Wen-Yan Zan,Fengwei Zhang
Transition metal-nitrogen-carbon (M-N-C) catalysts show great promise for converting CO₂ into valuable fuels and chemicals via electroreduction (CO₂RR). Nonetheless, controversy remains regarding which specific MNₓ coordination structure in M-N-C catalysts governs CO₂RR performance. We synthesized a series of Ni-NOMC catalysts with high specific surface area and varying NiN₃-Pyr site loadings using SBA-15 as a template, employing a small molecule condensation and pyrolysis strategy. Aberration-corrected scanning transmission electron microscopy (AC-STEM) and X-ray absorption spectroscopy (XAS) confirmed the presence of atomically dispersed Ni sites coordinated by pyrrolic nitrogen (NiN₃-Pyr). The Ni-NOMC-3 catalyst, with a higher NiN 3 -Pyr loading, achieved a remarkable CO Faraday efficiency (FE CO ) of 99.6% at −0.57 V vs. the reversible hydrogen electrode (RHE), while maintaining FE CO > 99% across a broad potential window (−0.17 to −0.97 V vs. RHE). Moreover, the ordered mesoporous structure of this catalyst enhances mass transport properties and optimizes active site accessibility, enabling a high CO partial current density of 157 mA·cm⁻² in a flow cell system. Theoretical simulations further reveal that the NiN₃-Pyr coordination structure exhibits superior catalytic performance for CO₂RR-to-CO compared to other possible NiN x configurations.
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NUCLEAR TECHNOLOGY
·
2025
·
IF 2
Qianwen Wang,Dingcheng Wang,Jinfeng Li,Bo Tian,Zhigang Li,Jianwei Zhang,Wenze Li,Nan Zhang,Yunchen Du,Hongtao Zhao
The extraction and recovery of uranium play a crucial role in ensuring the sustainable supply of nuclear energy and safeguarding environmental security. The ideal uranium adsorbent should have high adsorption capacity, excellent selectivity, and good reusability. In this study, by employing the strategy of using MIL-100(Fe) as an intermediate linker, the core shell, structured of Fe3O4@NiFe-LDH, was successfully accomplished via a solvothermal method. The as-prepared Fe3O4@NiFe-LDH shows great potential in the field of uranium adsorption.On one hand, MIL-100(Fe) can act as an iron source for NiFe-LDH, making the core-shell structure more stable. It was observed that after four adsorption-desorption cycles, the adsorption efficiency of Fe3O4@NiFe-LDH could still reach 75% in the fifth cycle. By contrast, materials without the MIL-100(Fe) intermediate layer exhibited a relatively lower adsorption cycle efficiency for three cycles. On the other hand, the porous structure of metal organic framework (MOF) doubles the specific surface area of Fe3O4@NiFe-LDH compared to Fe3O4/NiFe-LDH without a MOF intermediate layer.The abundant hierarchical pore structure further enhances the performance of Fe3O4@NiFe-LDH from 615.6 mg·g−1 of Fe3O4/NiFe-LDH(8:1) to 862 mg·g−1. Additionally, in-depth studies on adsorption kinetics and adsorption thermodynamics suggest that the adsorption process is more inclined to monolayer adsorption and is dominated by chemical adsorption, which is a spontaneous endothermic process. When conducting ion competition tests on the adsorbent, it was found that the adsorbent has high adsorption selectivity for U(VI) and good regeneration ability. Therefore, the addition of the intermediate MOF improves the adsorption capacity and stability of the material, indicating that Fe3O4@NiFe-LDH has potential advantages in practical applications.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2026
·
IF 5.4
Lin Luo,Zhiyuan Liu,Yue Pan,Tao Xu,Ang Xiao,Baolong Jiang,Weiting Yang,Yida Deng
To overcome the shortcomings of epoxy coatings in inadequate long-term barrier properties and lack of active corrosion inhibition at defect sites, we developed a self-healing epoxy coating by incorporating a MIL-100(Fe) nanocomposite loaded with benzotriazole (BTA), which was synthesized using solvothermal and solution impregnation methods. This multifunctional system provides robust barrier protection and alkaline-triggered self-healing capabilities. The composite enables alkaline-triggered BTA release, forming a protective film at damaged sites. The synthesized MIL-100@BTA nanocomposite exhibits a high surface area, thermal stability, and controlled BTA release. In simulated seawater, the MIL-100@BTA/EP coating maintained a low-frequency impedance modulus of 5.03 × 10⁹ Ω·cm² after 50 days, significantly outperforming pure epoxy. Scratch tests, electrochemical tests, scanning electron microscopy (SEM) and electron dispersive spectrum (EDS) analyses confirmed that the released BTA inhibits corrosion by forming a protective film at defect sites. This work presents an effective strategy for engineering high-performance and self-healing coatings.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2026
·
IF 4.5
Yujing Zhou,Yizhe Yang,Yinqi Sun,Zihao Wang,Hengbo Ding,Kai Liu,Weiguo Zhang,Songke Feng
To overcome the low nitrogen use efficiency (<40%) of conventional urea, this study utilizes the metal–organic framework MIL-100(Fe)—characterized by ultrahigh surface area and tunable mesoporosity—as a promising carrier for nano slow-release fertilizers with enhanced nutrient stability. Fourier transform infrared spectroscopy, thermogravimetric analysis, and Brunauer–Emmett–Teller measurements confirmed that urea was uniformly accommodated within the MOF channels in an amorphous, physically adsorbed state without chemical bonding. High-performance liquid chromatography revealed that loading capacity was primarily determined by the urea-to-MOF mass ratio, whereas loading temperature and duration had negligible effects, enabling precise synthesis control. Orthogonal optimization identified the optimal parameters (mass ratio 1:1, 110°C, 7 h), yielding a urea loading of 59.2% and encapsulation efficiency of 51.8%. Release experiments demonstrated a 22.5-fold extension in release duration compared to pure urea, with 87.6% cumulative release over 180 h governed by Fickian diffusion. Furthermore, physical characterization and bench-scale metering tests verified the granules' mechanical adaptability, achieving stable, continuous discharge comparable to urea. This work validates MIL-100(Fe)@UREA as a high-capacity, mechanically viable platform for sustainable and precision nutrient delivery. These results not only highlight the potential of MIL-100(Fe) in advanced slow-release fertilizer systems but also provide valuable insights for designing efficient and environmentally sustainable nutrient delivery platforms.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 26
·期 3
·1625-1629
·
IF 3.3
Yang Li,Jiating Wu,Yuhe Zheng,Yajing Fan,Ting Bian,Xinyu Fan,Santana Vimbai Masendu,Junhua Xu,Zongping Shao
Photocorrosion is the most ticklish problem of cuprous oxide (Cu2O), and it is widely assumed that the deactivation of Cu2O photocathodes in solar water splitting is caused by spontaneous oxidation–reduction (REDOX) reactions. However, this work shows that 〈100〉-oriented Cu2O photocathodes undergo a non-REDOX hydration deactivation mechanism. Briefly, water molecules are embedded in the Cu2O crystals at low potential under illumination and produce amorphous CuOH, which can be dehydrated at high potential to heal the Cu–O–Cu bonds and regenerate foamed Cu2O films with a three-dimensional skeleton structure. This study provides a new insight towards the protection and application of Cu2O photocathodes.
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TURKISH JOURNAL OF CHEMISTRY
·
2024
·Vol. 47
·期 6
·1307-1319
·
IF 1.3
WANG YUN-DONG,CHEN YI-JUN,CHENG MEI-NA,LIU XIN
In this paper, a novel Fenton reaction system which was called MHACF-MIL-100(Fe) was constructed. In this system, based on active hydrogen-accelerated FeIII reduction, the hydroxyl radical was continuously produced with a trace amount of total iron. The MIL-100(Fe) modified with the nano-Pd0 particle could be used to activate the H2. Under normal temperature and pressure, the target organic pollutants, such as sulfamethazine and 4-chloro phenol, could be degraded fast. In the condition of initial aqueous solution pH 3, 2 g L–1 dosage of MIL-100(Fe) catalyst loaded with nano-Pd0, Pd/MIL-100(Fe), 20 mM 30 wt% hydrogen peroxide, 25 μM ferrous chloride and 60 mL H2 min–1, 97.8% of sulfamethazine and 100% 4-chloro phenol could be degraded within only 5 min, respectively. Although the surface of the catalyst exhibited more obvious defects and roughness after 5 consecutive destructive experiment cycles, its basic structure could be maintained. The removal efficiency could be maintained at least more than 79% (sulfamethazine) and 94% (4-chloro phenol). That may be mainly attributed to the degradation of hydroxyl radical.
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