RARE METALS
·
2026
·Vol. 45
·期 5
·e70350
·
IF 12.1
Lijuan Wang,Jie Hou,Wubo Wan,Yongjie Mo,Zhijian Liao,Shengkui Zhong,Linhua Zhu
en This link goes to a English section zh This link goes to a Chinese section Atomically dispersed iron–nitrogen–carbon (Fe-N-C) catalysts have emerged as promising alternatives for oxygen reduction reaction (ORR) owing to their highly atomic utilization. However, maintaining both Fe atomic dispersion and dense Fe-N x sites (typically below 2 wt%) in Fe-N-C catalysts is still a key challenge. In this investigation, a template (1,2-dicyanobenzene; DCB) assisted strategy has been reported to achieve hierarchically porous Fe-N/C DCB0.2 -900°C catalysts, which have atomically dispersed Fe-N 4 C active sites with a 5.45 wt% Fe loading and served for robust ORR. 1,2-dicyanobenzene containing abundant nitrogen source not only efficiently enhances the coordinated environment for dense Fe sites, but also facilitates the formation of a hierarchical porous structure in Fe-N/C DCB0.2 -900°C catalyst. Computational analysis demonstrated that template-assisted structural modification effectively reduces the energy barrier associated with *OOH intermediate formation while simultaneously adjusting the d-band center position of Fe-N 4 C coordination sites within the Fe-N/C DCB0.2 -900°C system. This optimization enhances the stabilization of oxygen-bearing intermediates and promotes accelerated kinetics of the ORR. Consequently, the Fe-N/C DCB0.2 -900°C exhibited a half-potential of 0.9 V versus RHE when evaluated in 0.1 M KOH electrolyte and achieved a peak power density of 220 mW cm −2 in a zinc–air battery, surpassing commercial Pt/C (0.88 V vs. RHE, 194 mW cm −2 ). Such methodology provides a new avenue for constructing dense metal active sites for achieving functional, but not limited to, ORR, catalysts and applications. 摘要 en This link goes to a English section zh This link goes to a Chinese section 原子分散的铁-氮-碳(Fe-N-C)催化剂因其高原子利用率,已成为很有前景的氧还原反应(ORR)替代催化剂。然而,在Fe-N-C催化剂中同时保持铁的原子分散性和密集的Fe-N x 位点(通常低于2 wt%)仍是一个关键挑战。在本研究中,我们报道了一种模板(1,2-邻苯二甲腈; DCB)辅助策略,以制备具有分级多孔结构的Fe-N/C DCB0.2 -900°C催化剂,该催化剂具有原子分散的Fe-N 4 C活性位点,铁负载量为5.45 wt%,可用于高效的ORR。含有丰富氮源的1,2 -邻苯二甲腈不仅能有效改善密集铁位点的配位环境,还有助于在Fe-N/C DCB0.2 -900°C催化剂中形成分级多孔结构。理论计算分析表明,模板辅助的结构修饰有效降低了与*OOH中间体形成相关的能垒,同时调整了Fe-N/C DCB0.2 -900°C体系中Fe-N 4 C位点的d带中心位置。这种优化增强了含氧化合物中间体的稳定性,并促进了ORR的动力学反应速度。因此,在0.1 M KOH电解质中测试时,Fe-N/C DCB0.2 -900°C的半波电位为0.9 V,在锌空气电池中实现了220 mW cm −2 的峰值功率密度,超过了商用Pt/C(0.88 V,194 mW cm −2 )。这种方法为构建密集的金属活性位点提供了新途径,可用于制备功能性催化剂(不仅限于ORR)及相关应用。
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高影响因子
Journal of Materials Chemistry A
·
2026
·
IF 9.2
Hamza M. Haruna,Yanxiang He,Zhixiao Zhu,Hao Yang,Selvam Mathi,Guanhua Zhang,Zhongmin Wang,M. Sadeeq Balogun
Controlling phase evolution during nitridation is essential for creating active interfaces in multi-metal electrocatalysts. However, the nitridation pathways in complex systems such as Mo-Fe-Ni molybdates remain poorly defined. Herein, tuning the Fe contents in the Fe-Mo precursor directly governs ammonia activation and drives nitridation-induced reconstruction. Increasing Fe concentration promotes NH3 decomposition, shifting the product from an oxide-rich phase (N-doped MoO2-FeMoO4-NiMoO4-NiO, denoted N/MoO2-MoFeNi-O) to a nitride-dominated heterostructure comprising MoO2, Mo2N, FeN and Ni4N (N/MoO2-MoFeNi-N). The optmized N/MoO2-MoFeNi-N nitride-oxide interfaces enhance electrical conductivity, optimize oxygen-intermediate adsorption, and improve corrosion resistance. As a result, N/MoO2-MoFeNi-N exhibits superior oxygen evolution performance in both alkaline freshwater and seawater, requiring overpotentials of only 309/392 and 334/499 mV to reach 500 and 1000 mA cm-2, respectively. DFT calculations identify the MoO2@FeN interface is the most active site with the lowest energetic barrier for the potential-limiting step. The catalyst also demonstrates efficient oxygen reduction activity, enabling high-performance zinc-air batteries with open-circuit voltage of 1.33 V, peak power density of 84.2 mW cm-2, and stable cycling over 140 h. This work clarifies the role of Fe in directing nitridation pathways, providing a rational route to construct durable, interface-rich nitride-oxide architectures for advanced oxygen atalysis.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Wenqiang Cao,Xiyu He,Xiyang Cai,Qiaodan Hu,Junliang Zhang,Fan Yang
Electrocatalytic nitrate reduction offers a sustainable approach to ammonia synthesis while simultaneously addressing nitrate contamination. Electrocatalysts with high activity, long durability and affordable cost are essential for advancing this field. This study demonstrates that Fe-doped TiO 2 nanoparticles synthesized by a simple hydrothermal route exhibit competitive electrocatalytic performances for nitrate-to-ammonia conversion. A faradaic efficiency (FE) of 82.3 %, an ammonia yield of 5.953 mg·cm −2 ·h −1 , and a selectivity of 85 % can be achieved and maintained in 10 cycles with a total duration of 60 h in alkaline electrolyte. These metrics substantially outperform the pristine TiO 2 . Defect chemistry analysis and DFT calculations reveal that Fe doping creates oxygen vacancies, and introduces impurity energy levels in the bandgap to improve the electrical conductivity of TiO 2 . Fe and oxygen vacancies synergistically modulate the nitrate adsorption energy, and the Fe active site further reduces the energy barrier for the rate-limiting step and suppresses the competing reactions, thereby effectively promoting ammonia synthesis.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 9
·092522
·
IF 4.386
Jian-Ru Li,Cun-Ying Xu,Jing-Ling Lu,Shu-Xian Wang,Xiao Chen,Qin-Qin Xiang,Yi-Xin Hua
The electrodeposition behavior of Fe was studied in phenyltrimethylammonium chloride-ethylene glycol eutectic-based ionic liquids (TMPAC-EG EILs) containing FeCl2 through electrochemical measurement and the deposit characterization. Some kinetic parameters (standard rate constants, transfer coefficients and activation energy for standard rate constants) as well as transport properties were obtained and discussed as function of temperature. The values of transfer coefficient (0.32–0.39) are significantly lower than conventional value (0.5). Electrodeposition of Fe follows three-dimensional progressive nucleation and growth mode, which is unaffected by temperature. Besides, it is found that deposition temperature plays a central role in controlling surface morphology and structure of the resultant Fe coatings. At low temperature (333–353 K), smooth and dense iron coating can be obtained. The phase structure changes from a nanocrystalline α-Fe to amorphous phase (metallic glass) as the deposition temperature increases from 333 K to 353 K.
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Advanced Science
·
2021
·Vol. 8
·期 22
·2101824
·
IF 16.806
Jun Wang,Bin Li,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Wenchao Peng
Fenton-like reactions with persulfates as the oxidants have attracted increasing attentions for the remediation of emerging antibiotic pollutions. However, developing effective activators with outstanding activities and long-term stabilities remains a great challenge in these reactions. Herein, a novel activator is successfully synthesized with single iron atoms anchored on porous N-doped carbon (Fe-N-PC) by a facile chemical vapor deposition (CVD) method. The single Fe atoms are coordinated with four N atoms according to the XANES, and the Fe-N 4 -PC shows enhanced activity for the activation of peroxymonosulfate (PMS) to degrade sulfamethoxazole (SMX). The experiments and density functional theory (DFT) calculations reveal that the introduction of single Fe atoms will regulate the main active sites from graphite N into Fe-N 4 , thus could enhance the stability and tune the PMS activation pathway from non-radical into radical dominated process. In addition, the N atoms connected with single Fe atoms in the Fe-N 4 -C structure can be used to enhance the adsorption of organic molecules on these materials. Therefore, the Fe-N 4 -C here has dual roles for antibiotics adsorption and PMS activation. The CVD synthesized Fe-N 4 -C shows enhanced performance in persulfates based Fenton-like reactions, thus has great potential in the environmental remediation field.
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PubMed
高影响因子
Chemical Engineering and Processing-Process Intensification
·
2021
·
IF 4.237
Dicka Ar Rahim,Wei Fang,Gaojun Zhu,Haryo Wibowo,Dwi Hantoko,Qing Hu,Herri Susanto,Zengliang Gao,Mi Yan
Before syngas from gasification of biomass could be used as synthesis fuel or chemical feedstock, it requires the removal of hydrogen sulfide (H 2 S) to meet the purity standard level of those applications. In this study, Zn-Fe/Al 2 O 3 were successfully synthesized by a microwave-assisted wet incipient impregnation technique for use as adsorbent for H 2 S removal. The characterization of synthesized adsorbents showed that the oxide form of Zn and Fe present on the surface of adsorbents were zinc oxide (ZnO), magnetite (Fe 3 O 4 ), and zinc ferrite (ZnFe 2 O 4 ). While the reduction of adsorbent was mostly due to that of iron oxide . The reduced adsorbents might consist of ZnO/Fe 3 O 4 /FeO/Fe on alumina as support. At relatively high space velocity (26,000 h −1 ) the adsorbents were able to reduce the H 2 S concentration from 250 ppm at the inlet to around 45 ppm, 35 ppm, and 25 ppm at the outlet by adsorbent 1ZnFe, 2ZnFe, and 3ZnFe; respectively. The removal efficiency for adsorbent 1ZnFe, 2ZnFe, and 3ZnFe were 82%, 86%, and 90%; respectively. Results also shown an increase in adsorbent lifetime with the increase of the Zn to Fe ratio.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Ziyi Xiao,Rui Wu,Tingting Shu,Yingxi Wang,Ling Li
In order to further improve the catalytic performance of MIL-101, cobalt-doped MIL-101(Fe,Co) was synthesized by solvothermal method. By adjusting the ratio of cobalt doping, the MIL-101(Fe,Co 20% ) with the best catalytic activity was obtained. The activation performance of MIL-101(Fe,Co 20% ) for peroxymonosulfate (PMS) was studied using Rhodamine B (RhB) as a pollutant model. The experimental results proved MIL-101(Fe,Co 20% ) with much better catalytic performance than MIL-101(Fe), which can degrade more than 99% of RhB within 15 min. The effects of initial solution pH and coexisting anions in water on the degradation of RhB were further discussed. The results showed that MIL-101(Fe,Co 20% ) was with excellent stability and degradation efficiency can still keep above 90% after five cycles. The free radical quenching experiments were further studied to explore the degradation mechanism. It can be concluded that SO 4 - · was the main active free radical for the degradation of RhB. The possible intermediate products in the degradation process of RhB were analyzed by LC-MS. Combined with the comparison of XPS before and after the reaction, the possible reaction mechanism of RhB degradation process was inferred.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Zibin Pan,Zhengxian Chen,Gary Owens,Zuliang Chen
Biosynthesis strategies are promising methods for the sustainable preparation of nanoparticles because they are less toxic to living organisms and the environment. However, there are still several knowledge gaps concerning the exact mechanisms involved in the biosynthesis of bimetallic composites when used for the removal of arsenic species. Thus, this work focused on the biosynthesis mechanism involved in the formation of a Fe/Cu bimetallic bio-composite (Fe/Cu-OC), and determination of the specific biomolecules in tea extract involved in biosynthesis, and identification of the reactive sites involved in the removal of As(V). FTIR , XPS, GC-MS, and LC-MS analysis of the main components of the tea extract proved that the surface of Fe/Cu-OC contained many different functional groups, including -OH, Fe/Cu-O, and O C-OH, which were mainly associated with theanine and caffeine complexes. SEM and TEM analyses indicated that Fe/Cu-OC had both crystalline and amorphous features with an average particle size of 366 ± 10 nm. A 97 % removal efficiency for As(V) was obtained by Fe/Cu-OC, suggesting that the surface contained numerous reactive sites, including unsaturated Fe and Cu complexes, as well as saturated benzene rings. Moreover, DFT calculations indicated that the Gibbs free energy changes for the preparation of Fe/Cu-OC were < 0, suggesting that in the composites biosynthesis was a thermodynamically favored spontaneous reaction. A biosynthetic mechanism for the formation of Fe/Cu-OC was proposed, involving a series of spontaneous coordination, redox, and organic adsorption reactions.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Guolong Lu,Xin Men,Ruoqi Tang,Zhida Wang,Hao Cui,Tongxi Zheng,Mi Wang,Haoqi Yang,Zhenning Liu
Transition metal and nitrogen co-doped carbon electrocatalysts are promising candidates to replace the precious metal platinum (Pt) in oxygen reduction reactions (ORR). Unfortunately, the electrochemical performance of existing electrocatalysts is restricted due to limited accessibility of active sites. Inspired by jellyfish tentacles, we design an efficient ORR micro-reactor called Fe-N x /HC@NWs. It features abundant exposed Fe-N x active sites dispersed on nitrogen-doped cubic carbon cages, which have a hierarchically porous and hairy structure. The accessible, atomically dispersed Fe-N x sites and the elaborate substrate architecture synergize to provide the catalyst withremarkable ORR catalytic activity, extraordinary long-term stability, and favorable methanol tolerance in an alkaline electrolyte ; overall, its performance is comparable to that of commercial carbon-supported Pt. Our synthesis is facile and controllable, paving a new avenue toward advanced non-precious metal-based electrocatalysts for energy storage and conversion .
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PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
·
IF 11.4
Yanjing Wang,Minglei Song,Jianrong Wei,Jie You,Siping Chen,Shuangyin Wang,Yanyong Wang
Electrochemically mediated Fe(II)/Fe(III) redox-coupled uranium extraction can efficiently reduce the cell voltage of electrochemical uranium extraction (EUE). How to regulate the surface structure to enhance the uranium acyl ion adsorption capacity and strengthen the Fe(II)/Fe(III) redox cycle process is crucial for EUE. In this work, we developed surface sulfated nanoreduced iron (S-NRI) for EUE and exhibited improved properties for EUE at an ultralow cell voltage (−0.1 V). Compared with a nanoreduced iron (NRI) adsorbent, S-NRI displayed faster electrochemical extraction kinetics properties and higher extraction efficiency and capacity for uranium. In a more complex seawater electrolyte containing uranyl ion concentration ranging from 1 to 20 ppm, the removal efficiency could reach almost ∼100% after EUE for 24 h. At a higher 50 ppm uranium acyl ion concentration in a seawater electrolyte, S-NRI exhibited higher extraction capacity (755.03 mg/g), which is better than 528.53 mg/g of NRI at a cell voltage of −0.1 V. Outstanding EUE property could be attributed to the fact that sulfate species (M–SO42–) on the S-NRI surface not only enhanced selective adsorption of uranyl ions but also strengthened the Fe(II)/Fe(III) redox cycle, which accelerated electron transfer between Fe(II) and U(VI), promoted the regeneration of Fe(II) active sites, and finally enhanced the EUE property.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Dongping Zhang,Yongdi Liu,Yanyu Song,Xianbo Sun,Wen Liu,Jun Duan,Zhengqing Cai
A Fe-doped CeO 2 was fabricated for catalytic ozonation of Amoxicillin (AMX), and the catalytic mechanisms were explored in this study. Under optimal conditions (the initial solution pH of 7.0, FC-0.3 dosage of 0.5 g/L, O 3 dosage of 4 mg/min), the AMX and TOC removal by the optimal material (FC-0.3, at Fe/Ce atomic ratio of 0.3) reached 98.1 % at 24 min and 55.2 % at 36 min, respectively. Improved the AMX mineralization efficiency by 3.7 times. The experiments and theoretical calculation reveal the mechanisms of promoted catalytic ozonation by FC-0.3: 1) Highly abundant surface-active sites (i.e., –OH) enabled the adsorption of H 2 O and O 3 , which was favorable to the generation of reactive oxygen species (ROS) and improved the reaction probability for ROS and contaminants. 2) The synergistic effect between Ce 4+ /Ce 3+ and Fe 3+ /Fe 2+ redox couples accelerated the electron transfer and formation of ROS. More than 42 % of •OH was generated in the presence of FC-0.3, and the •OH, •O 2 − and 1 O 2 were the main ROS that contributed to AMX degradation. The surface OH groups played a key role in the catalytic ozonation. The oxygen vacancies (OVs) played an important role in electron transfer, Ce and Fe were the active sites of electrons transfer following the sequence of (Ce 3+ + Fe 2+ ) → (Ce 4+ + Fe 3+ ) → (Ce 3+ + Fe 2+ ) redox reaction. The degradation pathway investigation and toxicity evaluation revealed that some more toxic intermediates were generated during the ozonation process, and sufficient mineralization is required to meet safe discharge. This study provides reference for the synthesis of new catalysts and insight into the reaction mechanisms in the heterogeneous catalytic ozonation process.
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CHEMICAL GEOLOGY
·
2024
·
IF 3.6
Kuan Cheng,Zesheng Yang,Guojun Chen,Shiwen Hu,Chao Guo,Yang Yang,Shan Wang,Ying Wang,Haibo Dong,Milan Wang,Pengfei Cheng,Tongxu Liu
The nitrate-reducing Fe(II)-oxidizing (NRFO) process plays a crucial role in geochemical Fe N coupled cycling under anoxic conditions. Both nitrate and nitrite can act as electron acceptors for NRFO bacteria, resulting in the formation of Fe(III) minerals. Nevertheless, the stability of Fe(III) minerals generated during the NRFO process remains unclear. In this study, the Fe(III) minerals were obtained using the model NRFO bacteria strain Acidovorax sp. BoFeN1 in the presence of nitrate or nitrite. The stability of the Fe(III) minerals was examined in the presence of the model Fe(III) reduction bacteria Shewanella oneidensis MR-1 (strain MR-1), the chemical reducing reagent sodium dithionite (Na 2 S 2 O 4 ), and hydrochloric acid (HCl), respectively. The main Fe(III) minerals were goethite in the nitrate treatments (named M nitrate ) and tightly attached to the surface of cells. Meanwhile, the main Fe(III) minerals were lepidocrocite in the nitrite treatments (named M nitrite ), showing slight adherence to the cell surface. The reductive dissolution kinetics of M nitrate by strain MR-1 revealed a gradual increase in Fe(II). Little Fe(II) was formed when reduced M nitrite , which was attributed to the residual nitrite acted as a competitive electron acceptor to Fe(III), inhibiting the microbial Fe(III) reduction processes. Furthermore, the Fe(III) minerals were harvested by centrifugation and then reacted with sodium dithionite and hydrochloric acid (HCl), respectively. The incorporation of sodium dithionite and hydrochloric acid facilitated the dissolution of Fe(III) minerals. In the M nitrite treatments, the Fe(III) minerals exhibit enhanced stability due to their inherent higher crystallinity and the protective influence of cell surface and microbial carbon. This study broadens our understanding of the formation and transformation of microbial Fe(III) minerals, thereby improving our knowledge of biogeochemical iron cycling under anoxic conditions.
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