Chemical Science
·
2026
·
IF 8.1
Wenlong Zhang,Xiaohui Ning
The Fe/FeCl₂-Graphite battery is an intermediate-temperature molten salt electrochemical system. It employs the solid Fe/Fe2+ redox as the negative electrode reactions and graphite positive electrode based on the intercalation/de-intercalation reaction of AlCl- 4, offering high safety, low material cost and a moderate operating temperature range of 110-150 °C. However, the poor electronic conductivity and high nucleation barrier in the FeCl2 material result in limited electrochemical reversibility and reaction kinetics. Here, we demonstrate that the Fe-FeCl₂ contact interface effectively enhances the redox reversibility and electrode kinetics by providing favorable sites for Fe⁰ nucleation and improving electronic conductivity. The prepared Fe-FeCl₂-CR electrode delivers low voltage hysteresis of 0.09 V and exhibits excellent electrochemical reversibility in the Fe/FeCl₂-graphite molten salt battery, achieving a specific capacity of 162.6 mAh g⁻¹ at 3 mA cm⁻² and retaining 93% of its capacity after 200 cycles. Compared with the pure FeCl₂ electrode, the Fe-FeCl₂-CR electrode shows lower direct‑current pulse resistance and negligible nucleation overpotential, which are primarily attributed to the Fe‑philic nucleation interface. This mechanism is further confirmed by density functional theory (DFT) calculations, revealing that the (110) crystal plane of nano‑Fe possesses the highest binding energy (-55.94 eV) during charging, thereby serving as the potential dominant interface for Fe⁰ nucleation. Additional self‑discharge and capacity expansion tests further confirm the electrochemical reaction stability of Fe-FeCl₂-CR electrode in Fe/FeCl₂-Graphite molten salt battery.
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LANGMUIR
·
2026
·
IF 4.4
Yankun Wei,Dan Wang,Jinxiang Chou,Ruopeng Li,Wenchang Wang,Naotoshi Mitsuzaki,Zhidong Chen
Abstract Developing Fe–N–C electrocatalysts with high active site utilization remains a key challenge for the oxygen reduction reaction (ORR), primarily because of the limited accessibility of Fe-Nx sites. Herein, a hierarchically porous Fe–N–C (HP-Fe–N–C) catalyst is constructed via a ZnO-templated strategy combined with urea-assisted secondary pyrolysis, enabling the simultaneous regulation of the pore structure and Fe-Nx site density. The ZnO template governs the formation of mesoporous architectures, and concurrently, the pyrolysis of urea releases gaseous species that facilitate the enlargement and interconnection of mesoporous channels. Notably, the balanced micromesoporous structure derived from the ZnO template facilitates efficient mass transport and enhances site accessibility, while urea regulates the nitrogen species to promote the formation of dense Fe-Nx moieties. As a result, the HP-Fe–N–C catalyst delivers a high half-wave potential of 0.90 V, along with near four-electron selectivity and excellent durability. The Zn-air battery assembled with the HP-Fe–N–C cathode achieves an open-circuit voltage of 1.52 V, a specific capacity of 745.6 mAh g–1, and favorable charge–discharge stability exceeding 800 h. This work reveals the balance between hierarchical porosity and active site density in the Fe–N–C catalyst for the high-performance ORR.
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Results in Chemistry
·
2025
·
IF 4.2
Wei Zhang,Ku Yu,Wang Aihe
In this study, pyridine-a representative nitrogen-containing heterrocylic contaminant in coal chemical wastewater-was targeted for photocatalytic degradation. We developed a novel ternary composite photocatalyst through the in-situ integration of layered double hydroxide (LDH) and iron-based metal-organic framework (MIL-101(Fe)) with lanthanum‑iron co-doped TiO 2 via hydrothermal synthesis. These contaminants are characterized by high environmental persistence, low biodegradability, and potential teratogenic/carcinogenic risks. The synthesized LDH/MIL-101(Fe)/La-Fe-TiO 2 composite was systematically characterized using scanning electron microscopy (SEM), UV–Vis diffuse reflectance spectroscopy (DRS), X-ray photoelectron spectroscopy (XPS), and Brunauer-Emmett-Teller (BET) analysis. Key findings revealed that: (1) The composite architecture achieves an exceptional specific surface area of 168.96 m 2 /g through synergistic LDH/MIL-101(Fe) integration; (2) La–Fe co-doping effectively extends the photoresponse threshold of TiO 2 to the visible-light region. Under optimized conditions (25 °C, 300 rpm agitation, 400 W irradiation), the system achieved 96.1 % pyridine degradation (initial concentration: 100 mg/L) within 4 h, following pseudo-first-order kinetics (R 2 = 0.99). Remarkably, the catalyst maintained 94.5 % efficiency after five consecutive cycles, demonstrating superior stability. Mechanistic investigations combining GC–MS analysis, electron paramagnetic resonance (EPR) detection, and radical quenching tests identified the reactive species activity sequence as ∙ h + > ∙ OH > O 2 − , ultimately elucidating the complete pyridine mineralization pathway.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 42
·20490-20496
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IF 3.925
Ling Li,Jing Wu,Lieyuan Huang,Gaoli Lan,Naxiang Wang,Hui Zhang,Xin Chen,Xingbo Ge
Commercial applications of electrolytic water splitting require cost-efficient and active oxygen evolution catalysts. Nickel–iron (NiFe)-based compounds have attracted significant attention as oxygen evolution reaction (OER) catalysts due to their high catalytic activity. We develop a simple and easily controlled method by combining anodic fluoridation and cyclic voltammetry (CV) treatment to convert NiFe alloy to Ni/Fe hydroxide. A cracked layer structure of Ni/Fe hydroxide formed on the surface during the fluoridation of NiFe alloy and the CV process in KOH. The Ni/Fe hydroxide exhibits considerable OER activity with an onset potential of 1.47 V vs. RHE and a Tafel slope of 47 mV dec−1 in 0.1 M KOH. The electrode also shows an acceptable stability in alkaline media. The results indicate that anodic fluoridation and CV treatment are promising methods to form active layer structures of hydroxide on transition metals and their alloys, further increasing the electrocatalytic activity of the catalyst.
研究领域:
材料科学
·
电化学
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Journal of Cleaner Production
·
2023
·
IF 11.1
Hao Cheng,Xinyan Li,Chao Huang,Jian Zhu,Ping Wang,Heng Cao,Chongling Feng,Dingxun Ling,Hao Liu,Min Cheng
Commercial molybdenum carbide (Mo 2 C) and ferrous iron (Fe 2+ ) were investigated for the first time to co-catalyze the activation of H 2 O 2 for the treatment of organic contaminants . Compared with traditional Fenton process, the presence of Mo 2 C decomposed hydrogen peroxide (H 2 O 2 ) more effectively and accelerated the conversion of Fe 3+ /Fe 2+ . The Rhodamine B (RhB) degradation rate constant in Mo 2 C/Fe 2+ /H 2 O 2 reached appropriately three times that in Fe 2+ /H 2 O 2 , and the co-catalytic reactivity of Mo 2 C was significantly higher than that of MoS 2 . In addition, Mo 2 C/Fe 2+ /H 2 O 2 exhibited a board effective pH range of 2.8–8.8, and four-cycle experiments confirmed the stability and reusability of Mo 2 C. The results of X-ray photoelectron spectroscopy (XPS) indicated that Mo(Ⅱ) and Mo(IV) played major roles in Fe 3+ reduction. Electron Paramagnetic Resonance analysis and quenching experiments demonstrated that hydroxyl radical (·OH), superoxide anion radical (O 2 − ) and singlet oxygen radical ( 1 O 2 ) were all involved in Mo 2 C/Fe 2+ /H 2 O 2 . Particularly, Mo 2 C/Fe 2+ /H 2 O 2 significantly enhanced the generation of ·OH and 1 O 2 in comparison to Fe 2+ /H 2 O 2 . Moreover, toxicity assessment analysis by ECOSAR suggested that the toxicity of most degradation products of RhB decreased after treatment. Overall, this study offers a promising Mo 2 C co-catalyzed Fenton process for rapid and efficient abatement of organic contaminants.
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Journal of Cleaner Production
·
2022
·
IF 11.072
Yibing Xie,Mengyu Wang,Xueqian Wang,Langlang Wang,Ping Ning,Yixing Ma,Jichang Lu,Rui Cao,Yu Xue
The traditional way for arsine (AsH 3 ) removal from the reducing exhaust gas by catalytic oxidation undershot the expect goal in pollutant emission control. This laboratory scale work used magnetic field to improve the chemical environment of AsH 3 catalytic oxidation over magnetic response catalyst Fe/HZSM-5. After introducing external magnetic field at a magnetic field intensity of 0.1 T, the catalytic performance of Fe/HZSM-5 for AsH 3 removal was improved by 52%, and the turnover frequency (TOF) value increased from 4.65 × 10 −3 s −1 to 5.73 × 10 −3 s −1 . The structure–activity relationship of the catalyst in the presence of magnetic field was investigated. The characterization results showed that Fe is mainly anchored onto the surface of Fe/HZSM-5 catalyst through an oxygen bridge, while a small proportion of Fe exists in the form of iron oxides . The Fe species and surface labile oxygen (O − ) in the aluminum tetrahedra are the magnetic active sites of Fe/HZSM-5, magnetic field promotes the reaction by increasing the activity of them. It was discovered that paramagnetic O − increased by 50% in the presence of magnetic field compared with that in its absence. Therefore, a magnetic-field-assisted oxygen cycling process is proposed. In terms of the stability of catalyst, formation of more amorphous oxidized arsenic after reaction in the presence of magnetic field reduced the toxicity to the strong acid sites of the catalyst, and the holding time of excellent AsH 3 removal efficiency was prolonged from 23 h to 35 h. These results provide new insights into magnetic-field-assisted zeolite catalysis.
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WATER RESEARCH
·
2022
·
IF 13.4
Haolin Xu,Rundong Chen,Sheng Liang,Zhenchao Lei,Wenxiao Zheng,Zhang Yan,Jianxin Cao,Chaohai Wei,Chunhua Feng
The formation of chlorinated byproducts represents a significant threat to the quality of the effluent treated using electrochemical advanced oxidation processes (EAOPs), thus spurring investigation into alleviating their production. This study presents a new strategy to minimize the release of chlorinated intermediates during the electrochemical oxidation of Ni-EDTA by establishing a dual mixed metal oxide (MMO)/Fe anode system. The results indicate that the dual-anode system achieved a substantially higher rate (0.141 min − 1 ) of Ni-EDTA destruction and accordingly allowed a more pronounced removal of aqueous Ni (from 39.85 to 0.63 mg L − 1 ) after alkaline precipitation, compared with its single MMO anode (0.017 min − 1 of Ni-EDTA removal, with 14.38 mg L − 1 Ni remaining) and single Fe anode (insignificant Ni-EDTA removal, with 38.37 mg L − 1 Ni remaining) counterparts. Compared to reactive chlorine species (RCS) produced from the single MMO anode system, Fe(IV) was in situ generated from the dual-anode system and was predominantly responsible for the attenuation of chlorinated byproducts and thus the decrease in the acute toxicity of the treated solution (evaluated using luminescent bacteria). The Fe(IV)-dominated dual-anode system also exhibited superior performance in removing multiple pollutants (including organic ligands, Ni, and phosphite) in the real electroless plating effluent. The findings suggest that the strategy for Fe(II) transition to Fe(IV) by active chlorine paves a new avenue for yielding less chlorinated products with lower toxicity when EAOPs are used to treat chloride-containing organic wastewater.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Sihan Ma,Jun Xie,Lin Wang,Zonglang Zhou,Xian Luo,Jianghua Yan,Guang Ran
Photothermal/photodynamic therapy (PTT/PDT) and synergistic therapeutic strategies are often sought after, owing to their low side effects and minimal invasiveness compared to chemotherapy and surgical treatments. However, in spite of the development of the most PTT/PDT materials with good tumor-inhibitory effect, there are some disadvantages of photosensitizers and photothermal agents, such as low stability and low photonic efficiency, which greatly limit their further application. Therefore, in this study, a novel bismuth-based hetero-core–shell semiconductor nanomaterial BiNS–Fe@Fe with good photonic stability and synergistic theranostic functions was designed. On the one hand, BiNS–Fe@Fe with a high atomic number exhibits good X-ray absorption, enhanced magnetic resonance (MR) T2-weighted imaging, and strong photoacoustic imaging (PAI) signals. In addition, the hetero-core–shell provides a strong barrier to decline the recombination of electron–hole pairs, inducing the generation of a large amount of reactive oxygen species (ROS) when irradiated with visible–NIR light. Meanwhile, a Fenton reaction can further increase ROS generation in the tumor microenvironment. Furthermore, an outstanding chemodynamic therapeutic potential was determined for this material. In particular, a high photothermal conversion efficiency (η = 37.9%) is of significance and could be achieved by manipulating surface decoration with Fe, which results in tumor ablation. In summary, BiNS–Fe@Fe could achieve remarkable utilization of ROS, high photothermal conversion law, and good chemodynamic activity, which highlight the multimodal theranostic potential strategies of tumors, providing a potential viewpoint for theranostic applications of tumors.
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Materials Chemistry Frontiers
·
2021
·Vol. 5
·期 9
·3636-3645
·
IF 6.482
Xiaoqin Li,Taotao Gao,Qilin Liu,Yanxue Xu,Jing Li,Dan Xiao
Fiber-shaped energy storage devices (FESDs) are indispensable for developing portable and wearable electronic products. Aqueous rechargeable Ni/Fe batteries are an appropriate candidate due to the cost-effectiveness, high ionic conductivity, and great safety. However, their energy density is still far from satisfactory, hindering further practical applications. Herein, we focused on studying binder-free fibrous electrodes for high-performance FESDs based on rechargeable Ni/Fe batteries. A fast microwave-assisted synthesis method was adopted to grow active materials with a 3D conductive network which is constructed from carbon nanotubes decorated with Fe–Fe3C nanoparticles. Due to the heterogeneous structure, the active materials depicted improved electron/ion transfer, boosting the electrochemical performance of the anode. A flexible Ni/Fe battery is successfully fabricated using the aforementioned anode coupled with a NiCoO-based cathode which is synthesized by electrodeposition and a post-annealing process. Thanks to the special structure of the active materials and the fast redox reaction, the assembled flexible Ni/Fe battery achieved high electrochemical properties with a maximum volumetric specific capacity of 1.61 mA h cm−3 and energy density of 1.28 mW h cm−3. The cycling stability and mechanical flexibility were also tested, which demonstrated the prospects for practical application.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Cong Gao,Yan Su,Xie Quan,Virender K. Sharma,Shuo Chen,Hongtao Yu,Yaobin Zhang,Junfeng Niu
Heterogeneous Fenton-like reaction was a promising approach for generating •OH. However, the heterogeneous catalysts generally exhibited low activity because of slow reduction of Fe(III) in Fe(III)/Fe(II) redox cycle. Here, decreasing electron density was expected to quicken Fe(III) reduction and consequently enhance the catalytic activity of heterogeneous catalysts. This hypothesis was validated by the enhanced hydroxyl radicals generation and accelerated Fe(III) reduction on MIL-88B(Fe)-X (2-X-terephthalic acid, X = NH 2 , CH 3 , H, Br and NO 2 ) by reducing electron density of Fe(III) with substituent of higher electrophilicity. MIL-88B(Fe)-NO 2 , with the substituent of highest electrophilicity among these catalysts, has the lowest electron density of Fe(III) and highest redox potential ( E Fe(III)/Fe(II) = 0.35 V). As a result, it exhibited the best catalytic performance, which was 1.7–20 times higher than that for other MIL-88B(Fe)-X and was comparable to that of homogeneous Fe 2+ . This study provides scientific basis for rational construction of highly effective heterogeneous Fenton-like catalyst.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Xiaobing Wang,Chengyu Wei,Xiaosheng Song,Zuohui Wang,Yong Zhao
In the oxygen evolution reaction (OER), the non-reversible destruction of surface electronic structure caused by the irregular element migration in complex surface/interface reaction limits the improvement of catalyst’s activity and stability. Herein, we successfully realize the control of ‘dual-path migration of metallic elements in OER’ to stepwise reconstruct the O-coordinated bi-metal heterodimer (M 1 -O-M 2 ) for electron density redistribution. By designing Fe@FeNi 3 @NiO-Fe 3 O 4 (F-FN-NFO) model electrode with stepwise surface treatment in OER process, the directional migration (from core to shell, path 1 ) and adjacent-surface migration of Fe atoms ( path 2 ) are both controlled to reduce the formation energy of Ni-O-Fe units, realizing strengthened electron transfer between heterogeneous metal centers. After the surface reconstruction, the OER activity of F-FN-NFO increases for 8.6 times at 1.7 V (30.5–263 mA cm −2 ). Based on this strategy, the designed three-dimension NiFe@NiFe x O is positive activated compared to traditional NiFe-oxidation with the overpotential reduced to 299 mV at 10 mA cm −2 .
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CHEMOSPHERE
·
2023
·
IF 8.8
Chunsheng Ding,Xinze Song,Zhongyi Zheng,Hainan Wang,Yuqiang Pan,Hangtian Zhang,Xueyan Li,Jing Deng
Fe(II)-catalyzed PMS process was widely used in the degradation of refractory pollutants in wastewater, while its performance was restricted by the slow regeneration efficiency of Fe(II). Herein, caffeic acid (CFA), a representative of hydroxycinnamic acids, was introduced into Fe(III)/PMS system to accelerate the transformation of Fe(III) to Fe(II) and promote the removal of bisphenol A (BPA). Under optimum condition of 0.1 mM CFA, 0.05 mM Fe(III), and 0.5 mM PMS, almost complete removal of BPA can be achieved within 20 min, which was roughly 6.2 times higher than that in Fe(III)/PMS system. As the addition of CFA into Fe(III)/PMS system, pH application range was widened from acidic to alkaline conditions. The reduction and chelation of CFA expedited the Fe(III)/Fe(II) cycle by forming CFA-Fe chelate, thereby facilitating the PMS activation . Based on LC-MS analysis and DFT calculation, the intermediate products of CFA were found to play a decisive role in boosting the regeneration of Fe(II), and the toxicity of these intermediates towards organisms was evaluated by ECOSAR . The alcohol-scavenging and chemical probe tests certified that hydroxyl radical (•OH), sulfate radical (SO 4 •- ), and Fe(IV) coexisted in Fe(III)/CFA/PMS system, and the second-order reaction rate constants of •OH and SO 4 •- reacted with CFA were calculated to be 3.16✕10 9 and 2.30✕10 10 M −1 s −1 , respectively. Two major degradation pathways of BPA, •OH addition and SO 4 •- induced hydroxylation reaction, were proposed. This work presented a novel green phenolic compound that expedited the Fe(II)-catalyzed PMS activation process for the treatment of organic contaminants .
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