ACS Sustainable Chemistry & Engineering
·
2026
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IF 7.6
Jinjie Lin,Ce Gao,Xianhong Wu,Nan Wu,Run-Cang Sun
Abstract The electrocatalytic nitrate reduction reaction (NO3–RR) provides a sustainable and carbon-efficient strategy for ammonia (NH3) production, a vital industrial feedstock. However, the development of efficient electrocatalysts remains a significant bottleneck hindering its practical advancement. In alkaline media, effective electrocatalysts should not only activate nitrate but also promote water dissociation to supply proton equivalents for ammonia formation. Herein, we report the innovative application of sodium alginate (SA) hydrogels as a monolithic electrode for NO3–RR. The Fe3+ and Ni2+ ions coordinate with the carboxyl and hydroxyl groups in the sodium alginate to form a stable 3D porous network structure (FeNi/SA). In this structure, Ni sites promote water dissociation, whereas Fe sites facilitate nitrate reduction; the cooperation between these dual active sites accelerates ammonia formation. Consequently, the FeNi/SA hydrogel exhibits exceptional electrocatalytic performance, requiring potentials of only 0.0579 and –0.34 V (vs RHE) to achieve current densities of –10 and –100 mA cm–2, respectively. Notably, it delivers a high ammonia yield rate of 7.745 mg h–1 cm–2 with an impressive Faradaic efficiency of 93.79%. Experiment and density functional theory calculations results indicate that Ni sites promote the generation of *H and modulate the electronic structure of Fe, lowering the energy barrier for the critical *NO to *NOH transition and accelerating NH3 formation. Furthermore, integrating the NO3–RR process with an air-stripping system enables the efficient recovery of NH4Cl, offering a viable pathway for converting nitrogenous waste into high-value products. This work highlights the potential of hydrogel-based materials as a new frontier for robust nitrate-to-ammonia conversion.
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Small
·
2023
·Vol. 19
·期 43
·2302548
·
IF 13.3
Guangfeng Zeng,Dongjiang Chen,Cheng Zhen,Chao Feng,Yashuai Pang,Weidong He
Utilizing catalysts to accelerate polysulfides conversion are of paramount importance to eliminate the shuttling effect and improve the practical performance of lithium-sulfur (Li-S) batteries. The amorphism, attributes to the abundant unsaturated surface active sites, has recently been recognized as a contribution to increase the activity of catalysts. However, the investigation on amorphous catalysts has received limited interest in lithium-sulfur batteries due to lack of understanding of their composition structure activity. Herein, a amorphous Fe-Phytate structure is proposed to enhance polysulfide conversion and suppress polysulfide shuttling by modifying polypropylene separator (C-Fe-Phytate@PP). The polar Fe-Phytate with distorted VI coordination Fe active centers strongly intake polysulfide electron by forming Fe S bond to accelerate the polysulfide conversion. The surface mediated polysulfides redox gives rise to a higher exchange current in comparison with carbon. Furthermore, Fe-Phytate owns robust adsorption to polysulfide and effectively reduce the shuttling effect. With the C-Fe-Phytate@PP separator, the Li-S batteries exhibit an outstanding rate capability of 690 mAh g −1 at 5 C and an ultrahigh areal capacity of 7.8 mAh cm −2 even at a high sulfur loading of 7.3 mg cm −2 . The work provides a novel separator for facilitating the actual applications of Li-S batteries.
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CHINESE JOURNAL OF CATALYSIS
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2026
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IF 17.2
Xuebi Rao,Huiling Fang,Jialin Sun,Liqun Liu,Yongkang Zhu,Junxiang Chen,Shiming Zhang,Bin Liu
Noble-metal-free iron-nitrogen-carbon (Fe–N–C) catalysts with well-defined FeN 4 active sites are promising alternatives to replace platinum (Pt) catalysts for oxygen reduction reaction (ORR). However, the precise design of the peripheral heteroatom-doped FeN 4 centers and the clarification of the underlying electrocatalytic ORR mechanism remain a significant challenge. Herein, we employ a coordination engineering strategy to implant two sulfur (S) atoms into the second coordination shell of the FeN 4 center (FeN 4 S 2 ), which effectively modulates the Fe spin state via d z 2 - p , d xz - p , and d yz - p interactions. The symmetrical S-doping in FeN 4 S 2 can weaken the spin polarization of FeN 4 that induces a transition of single-Fe-atom from a high-spin to a medium-spin state, thereby optimizing the oxygen intermediates adsorption and transforming the ORR potential-determining step from *O → *OH over FeN 4 to *O 2 → *OOH over FeN 4 S 2 with a lower free energy barrier, which greatly boosts the ORR performance in both alkaline and acidic media. The zinc-air battery with a FeN 4 S 2 air electrode delivers a peak power density as high as 248.2 mW cm –2 with exceptional charge-discharge stability, significantly outperforming the state-of-the-art Pt/C air electrode.
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Journal of Energy Chemistry
·
2023
·
IF 13.1
Ruixue Zheng,Qinglei Meng,Hao Zhang,Teng Li,Di Yang,Li Zhang,Xiaolong Jia,Changpeng Liu,Jianbing Zhu,Xiaozheng Duan,Meiling Xiao,Wei Xing
Developing cost-effective, robust and stable non-precious metal catalysts for oxygen reduction reaction (ORR) is of paramount importance for electrochemical energy conversion devices such as fuel cells and metal-air batteries. Although Fe-N-C single atom catalysts (SACs) have been hailed as the most promising candidate due to the optimal binding strength of ORR intermediates on the Fe-N 4 sites, they suffer from serious mass transport limitations as microporous templates/substrates, i.e., zeolitic imidazolate frameworks (ZIFs), are usually employed to host the active sites. Motivated by this challenge, we herein develop a hydrogen-bonded organic framework (HOF)-assisted pyrolysis strategy to construct hierarchical micro/mesoporous carbon nanoplates for the deposition of atomically dispersed Fe-N 4 sites. Such a design is accomplished by employing HOF nanoplates assembled from 2-aminoterephthalic acid (NH 2 -BDC) and p -phenylenediamine (PDA) as both soft templates and C, N precursors. Benefitting from the structural merits inherited from HOF templates, the optimized catalyst (denoted as Fe-N-C SAC-950) displays outstanding ORR activity with a high half-wave potential of 0.895 V (vs. reversible hydrogen electrode (RHE)) and a small overpotential of 356 mV at 10 mA cm −2 for the oxygen evolution reaction (OER). More excitingly, its application potential is further verified by delivering superb rechargeability and cycling stability with a nearly unfading charge–discharge gap of 0.72 V after 160 h. Molecular dynamics (MD) simulations reveal that micro/mesoporous structure is conducive to the rapid mass transfer of O 2 , thus enhancing the ORR performance. In situ Raman results further indicate that the conversion of O 2 to *O 2 − the rate-determining step (RDS) for Fe-N-C SAC-950. This work will provide a versatile strategy to construct single atom catalysts with desirable catalytic properties.
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Journal of Inorganic and Organometallic Polymers and Materials
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2023
·
IF 4
Zhang Xue-Feng,Chang Tian-Long,Guo Na,Jia Guo-Liang,Li Xiao-Bing,Zhao Zhao-Ye,Wang Hui,Wang Jun-Chuan,Wu Xiang-Feng,Pan Cheng-Si,Liu Lei,Yang Lin-Lin
Fe-based MOFs (Fe-MOFs) are excellent photocatalysts and have synergy well with Fenton reagents relative to other MOFs. In this work, a series of uniformly covered NH 2 -Fe-MIL-88B@TpPa-1-COF composites were synthesized using an in-situ anchoring growth strategy, which used F127 as functional molecule to decorate NH 2 -Fe-MIL-88B nanoparticles to eliminate their surface electrostatic repulsion with Tp molecules during the subsequent coating procedure. Meanwhile, the -NH 2 groups in the skeleton of NH 2 -Fe-MIL-88B could also be used as anchors to covalently connect TpPa-1-COF shell and migration channels for effective charge transfer. This uniformly covered core–shell structure would endow these composites with much more contact area and imine bond linkage between the Fe-MOFs core and COFs shell. Compared with the random packing structure, the uniformly covered Fe-MOF@COF-3 composite possessed a higher proportion of Fe 2+ to Fe 3+ . As a result, the optimized Fe-MOF@COF-3 catalyst could achieve the highest photo-Fenton degradation efficiency of 93.9% for tetracycline hydrochloride (TC⋅HCl), which was much higher than 54.8% of pure NH 2 -Fe-MIL-88B. In addition, the uniform TpPa-1-COF shell could further effectively enhance the stability of NH 2 -Fe-MIL-88B by protecting Fe ions from leaching, and the toxicity of the water samples treated with our photo-Fenton degradation process declined obviously. All these merits will endow Fe-MOF@COF-3 photo-Fenton catalyst great potential application value as in the field of environmental governance.
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ACS Omega
·
2023
·
IF 4.1
Jun Li,Yuhang Hua,Qiannan Yuan,Wenqi Gou,Hao Sun,Long Lin,Mengtao Wang,Mingxun Yu,Aiwen Qin
A corolla-shaped Schiff base polymer was synthesized from terephthalaldehyde (TPAD), glutaraldehyde (GA), and p-phenylenediamine (PPD) by block copolymerization, and Schiff base iron complexes were formed by doping with FeCl3. The microscopic morphology, crystal structure, and elemental valence state were characterized by field emission scanning electron microscopy (FESEM), Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). Comparing the change of conductivity before and after Fe3+ doping, it was found that the conductivity did not break away from the category of insulator, and the doped sample is a paramagnetic material. Morphological changes were observed by adjusting the ratio of GA to TPAD, and it was found that the corolla-like structure was most complete when the ratio of GA to TPAD was 2:1, and its Schiff base iron complex absorbed waves better. At a thickness of 3 mm, the absorption effect can reach below −10 dB at 12.44–15.16 GHz, and the maximum absorption value is −45.07 dB at a thickness of 3.8 mm; it is an organic absorbing agent with excellent impedance matching and absorbing properties.
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CARBON
·
2023
·
IF 10.9
Zurong Zhu,Lu Zhang,Pinan Liu,Chengli Liu,Jialuo Ai,Youzhun Fan,Senwei Liu,Jinxia Zhai,Guanghui Bai,Chengyun Ning,Zhengao Wang
Excessive artificial electromagnetic radiation poses significant health risks and disrupts military equipment. To address this, high-performance microwave absorption materials are urgently required. While ferromagnetic materials have excellent absorption but suffer from high density, limited bandwidth , and perishable properties. Carbon materials, especially metal-organic frameworks (MOFs), offer promise due to low density, chemical stability, and high conductivity. In this study, we synthesized a novel multicore-shell Fe 3 O 4 @Fe@C composite via solvothermal and in-situ pyrolysis methods. This composite integrated Zn-MOF-derived porous carbon with core-shell Fe 3 O 4 @Fe@C, enabling multiple electromagnetic wave routes, strong interfacial polarization , and magnetic-dielectric synergy. It exhibited exceptional electromagnetic wave absorption, with a −59.1 dB reflection loss at 13.36 GHz and a 5.36 GHz effective absorption bandwidth. Our innovative MOF-core-shell approach holds great promise for highly efficient microwave absorbers to mitigate artificial electromagnetic radiation's adverse effects on health and military equipment.
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NEW JOURNAL OF CHEMISTRY
·
2023
·
IF 3.3
Guili Ge,Hanyu Tu,Dan Wang,Mingjian Chen,Zhaoyang Zeng,Can Guo,Xu Wu,Wei Xiong
Fe-CDs-PEG, leading to the occurrence of excess iron, iron metabolism disorder, GSH consumption, reactive oxygen species (ROS) accumulation, and activated the ferroptosis pathway, can enhance radiotherapy sensitivity by inducing ferroptosis in lung cancer cells. This study provides a new idea for effective therapy of lung cancer.
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ANALYTICAL SCIENCES
·
2023
·
IF 1.6
Yang Yu Meng,Yan Yuan,Zhou Jia Ying,Huang Cheng Zhi,Zhen Shu Jun,Zhan Lei
Real-time monitoring of hypochlorous acid (HClO) in biological systems is of great significance for exploring and regulating its pathological functions because abnormal production of HClO is closely related with many diseases, such as atherosclerosis, rheumatoid arthritis, and cancer. Herein, we developed a reliable fluorescent Fe-doped carbon dots (Fe-CDs) for the sensitive and selective detection of biological HClO using ferrocenecarboxylic acid and m -phenylenediamine as precursors through a one-step solvothermal procedure. The Fe-CDs exhibited excellent a wide HClO detection range from 20 nmol/L to 1000 nmol/L with corresponding limits of detection at 7.8 nmol/L. The sensing mechanism is based on the chemical oxidation of the hydroxyl groups on the surface of Fe-CDs by HClO. In addition, Fe-CDs also displayed high photoluminescence yield, excitation-independence emission, as well as good biocompatibility, enabling the successful imaging of endogenous and exogenous HClO in HeLa cells. These results revealed that Fe-CDs holds great promise as a robust fluorescent probe for investigating HClO-mediated biological events. Graphical abstract
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INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Naiyun Liu,Ruqiang Wu,Yixian Liu,Yunliang Liu,Peiji Deng,Yaxi Li,Yongchao Du,Yuanyuan Cheng,Zechao Zhuang,Zhenhui Kang,Haitao Li
Electrochemical nitrogen reduction reaction (NRR) is a promising method for ammonia synthesis under ambient conditions. However, the NRR performance is limited to an extremely strong N≡N bond in N2 and the competing hydrogen evolution reaction. Introducing oxygen vacancies (OVs) has been considered as a forceful means to accelerate the sluggish NRR reaction kinetics. Herein, we reported the design of Fe-doped NiMoO4 catalysts for NRR. Fe doping can increase the amount of OVs in the catalyst and contribute to lattice strain enhancement, thereby leading to the improvement of the electron transport rate and catalytic active for NRR. In 0.1 M Na2SO4 solution, the 5% Fe-NiMoO4 catalyst achieves a NH3 yield rate of 15.36 μg h–1 mgcat.–1 and a Faradaic efficiency of 26.85% under −0.5 V versus RHE. Furthermore, the 5% Fe-NiMoO4 catalyst exhibits excellent stability (up to 13 h) during the reaction.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Ying Wang,Gareth R. Williams,Yilu Zheng,Honghua Guo,Shiyan Chen,Rong Ren,Tong Wang,Jindong Xia,Li-Min Zhu
One of the major challenges in effective cancer therapy arises because of the hypoxic microenvironment in the tumor. This compromises the efficacy of both chemo- and radiotherapy , and thus hinders patient outcomes. To solve this problem, we constructed polydopamine (PDA)-cloaked Fe-based metal organic frameworks (MOFs) loaded with d -arginine ( d -Arg), glucose oxidase (GOX), and the chemotherapeutic drug tirapazamine (TPZ). These offer simultaneous multifaceted therapy combining chemodynamic therapy (CDT)/radiotherapy (RT)/starvation therapy (ST)/gas therapy (GT) and chemotherapy. The particles further can act as contrast agents in magnetic resonance imaging. GOX catalyses the conversion of endogenous glucose and O 2 to hydrogen peroxide and gluconic acid , blocking the cells’ energy supply and providing ST. With the resultant acidification of the local environment, the breakdown of the MOF releases TPZ (for chemotherapy) and Fe 3+ , which reacts with H 2 O 2 to produce reactive oxygen species and thus stimulates the conversion of d -Arg to NO for GT and RT sensitization. The PDA coating not only seals the pores and chelates Fe 3+ to enhance the T 1 -weighted magnetic resonance imaging (MRI) properties, but also is used to graft folate bovine serum albumin (FA-BSA) and thereby target the tumor site. The combined administration of low doses of X-ray irradiation and nanoparticles reduces the side effects on healthy tissue and can prevent lung metastases in mice. This work highlights the synergistic treatment of osteosarcoma via ST/GT/CDT/RT/MRI/ chemotherapy using a PDA-cloaked MOF system.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Xukai Li,Weirui Chen,Dongpo Liu,Gaozu Liao,Jing Wang,Yiming Tang,Laisheng Li
Due to its low interfacial electron migration ability and highly hydrophilic, Fe-MCM-41 (FeM) had poor activity and stability during catalytic ozonation . To this end, the secondary metal Zn and Si-F group were introduced into the framework of FeM to create surface potential difference and hydrophobic sites. Comparative characterizations showed that there existed rich acid sites with great potential difference on F-Fe-Zn-MCM-41 (FFeZnM). Additionally, because of the existence of hydrophobic and electron-withdrawing Si-F unit, the electron migration ability, hydrophobicity and acidity of FFeZnM were enhanced. The greater O 3 mass transfer was induced by Si-F group and O 3 was directly activated at Fe and Zn Lewis acid sites into •OH, •O 2 - and 1 O 2 . With •OH acting as main species, FFeZnM/O 3 achieved the superior IBP removal (93.4%, 30 min) and TOC removal (46.6%, 120 min) over those of sole O 3 and F-FeM/O 3 processes, respectively. HCO 3 - , Cl - , NO 3 - and SO 4 2- hindered IBP degradation by FFeZnM/O 3 , but high concentration humic acid (HA) exhibited promotion by forming HA-IBP complex. IBP degradation by FFeZnM/O 3 was enhanced with tap water , river water, and effluent from the secondary sedimentation tank of the sewage plant acting as medium. This study proposed an innovative approach to catalyst design for catalytic ozonation.
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