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Catalysts · 2023 ·Vol. 13 ·期 6 ·948 · IF 3.9

Nano-Hollow Zeolite-Encapsulated Highly Dispersed Ultra-Fine Fe Nanoparticles as Fischer–Tropsch Catalyst for Syngas-to-Olefins

Rui Hu,Tianye Wang,Yifan Wang,Yuan Zhu,Li Xie,Enhui Xing,Yu Wu,Zhijian Da

A nano-hollow zeolite-encapsulating ultra-fine Fe nanoparticle catalyst denoted as Fe@n-hS-HT was successfully synthesized through a simple water steam treatment of the Fe@n-hS catalyst prepared by the “dissolution–recrystallization” (D-R) method. The Fe@n-hS-HT catalyst had a hierarchical porous structure and a high dispersion of Fe2O3particles with a size of 3.4 nm. Furthermore, the results of several characterization methods, such as XRD, HAADF-STEM, and H2-TPR, further demonstrated the transformation of the skeleton Fe in Fe@n-hS into Fe2O3, which was uniformly dispersed in the Fe@n-hS-HT catalyst. Meanwhile, Fe@n-hS-HT had significantly higher selectivity and yield of C2-C4=than the reference catalysts Fe/S and Fe@n-hS, which provided strong proof for the confined catalysis of the metal@zeolite catalyst.Keywords:hollow zeolite;Fischer–Tropsch synthesis;encapsulation;iron catalyst

研究领域: 化学工程 · 催化科学
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ChemSusChem · 2016 ·Vol. 9 ·期 11 ·1339-1347 · IF 7.116

Catalytic Transfer Hydrogenation of Furfural to Furfuryl Alcohol over Nitrogen-Doped Carbon-Supported Iron Catalysts

Jiang Li,Jun-ling Liu,Hong-jun Zhou,Yao Fu

Graphical FF to FFA with Fe : Efficient catalytic transfer hydrogenation of furfural (FF) to furfuryl alcohol (FFA) over heterogeneous iron catalysts is demonstrated for the first time. Iron cations coordinated by pyridinic nitrogen functionalities on the carbon support are possibly responsible for the enhanced catalytic activity. This paves the way for achieving biomass conversion through heterogeneous iron catalysis. Iron-based heterogeneous catalysts, which were generally prepared by pyrolysis of iron complexes on supports at elevated temperature, were found to be capable of catalyzing the transfer hydrogenation of furfural (FF) to furfuryl alcohol (FFA). The effects of metal precursor, nitrogen precursor, pyrolysis temperature, and support on catalytic performance were examined thoroughly, and a comprehensive study of the reaction parameters was also performed. The highest selectivity of FFA reached 83.0 % with a FF conversion of 91.6 % under the optimal reaction condition. Catalyst characterization suggested that iron cations coordinated by pyridinic nitrogen functionalities were responsible for the enhanced catalytic activity. The iron catalyst could be recycled without significant loss of catalytic activity for five runs, and the destruction of the nitrogen–iron species, the presence of crystallized Fe 2 O 3 phase, and the pore structure change were the main reasons for catalyst deactivation.

研究领域: 化学工程 · 催化科学 · 生物质转化
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Sustainable production of carbon nanomaterials based on TPT backsheet pyrolysis from end-of-life photovoltaic modules

Luya Shen,Haoyang Li,Xi Yang,Shaoyuan Li,Yuelong Yu,Jijun Lu,Fengshuo Xi,Wenhui Ma,Rong Deng

The environmentally friendly recycling of end-of-life (EoL) photovoltaic modules is a crucial pathway to achieving “carbon neutrality.” However, currently, most efforts are primarily focused on the recovery of valuable metals, neglecting the utilization of TPT (Tedlar/PET/Tedlar) plastic backsheet. This work develops a two-stage pyrolysis process for TPT decomposition and which can convert into high-value nanocarbon materials and hydrogen under the catalysis of Ni and Fe nanometal particles. The pyrolysis behavior of TPT backplates was systematically investigated, the gas chromatography results reveal that the pyrolysis products primarily consisted of CO 2 , CO, CH 4 , CH 3 CHO, and other small molecules, alongside sizeable residual compounds under the catalytic degradation process. The resulting hydrocarbons play an important role as carbon sources in the formation of carbon nanomaterials and hydrogen generation. The study thoroughly discusses the effects of different catalyst on pyrolysis gas species and components, fixed carbon content, and nanocarbon morphology. Molecular dynamics simulations based on the reactive force field (ReaxFF) was performed to analyze the pyrolysis products. Finally, a gas–liquid-solid physical model was proposed to interpret the growth process of the carbon nanomaterials under Ni-Fe nanometallic catalysis.

研究领域: 环境科学 · 材料科学 · 能源科学
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Macromolecular Reaction Engineering · 2023 ·Vol. 17 ·期 3 ·2300013 · IF 1.5

Alkylaluminum/Urea Hybrid Cocatalysts and Their Use in Iron-Catalyzed Oligomerization of Ethylene

Ying Zhang,Jian Ye,Yinzhi Jiang,Shuqin Jiang,Wei Xiao,Dongchu Wei

The bis(imino)pyridyl iron-based ethylene oligomerization catalysts have the advantages of mild reaction conditions, high activity and high selectivity to linear α -olefins. However, barriers, such as high polymer content in the product mixture and large methylaluminoxane (MAO) dosage, are still limitations for the development of these systems at the industrial scale. In this study, new cocatalysts are prepared by the reaction of alkylaluminums with urea and its derivatives, and successfully used to activate iron-based catalysts. It is found that the type and molar ratio of alkylaluminum and urea have significant influence on the performance of the cocatalysts. The activity of the preferred triisobutylaluminum/urea activated systems reaches more than 3.0 × 10 8 g (mol-Fe) −1 h −1 , and the polymer content can be controlled to be less than 2 wt.%. Notably, the catalytic system exhibits good high temperature stability, the activity can still reach 1.0 × 10 8 g (mol-Fe) −1 h −1 even at 120 °C. Further 1 H NMR studies show that alkylaluminum can react with the N  H moieties of urea, forming complex alkylaluminum clusters, even aluminoxane-like structures. This study offers a promising family of cocatalysts, making it possible to simultaneously improve their performance and reduce their cost.

研究领域: 催化化学 · 材料科学
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Molecular Catalysis · 2025 · IF 4.9

Magnesium-doped Nickel-iron (Hyro)oxides-based Catalyst for Efficient and Stable Hydrogen Evolution

Jiaqi Feng,Wenwen Zhang,Kai Zhang,Hongyu Wang,Changcheng Wu,Jingde Li

NiFe-based materials offer tailorable electronic structure and exhibit promising performance in alkaline hydrogen evolution reaction (HER). Electron-rich earth metals as doping species can regulate the local electronic configuration of NiFe-based catalysts towards improved HER activity. Herein, a low electronegative Mg dopant strategy is utilized to prepare Mg-FeOOH/NiFeO x electrocatalyst for HER. The introduction of Mg improves the bonding strength of Fe-O bond in FeOOH active species, resulting in rapid H 2 O dissociation and improved stability. Meanwhile, Mg-dopant induces a downshift in the d -band center of FeOOH, which weakens the hydrogen adsorption for promoted H 2 production. The Mg-FeOOH/NiFeO x catalyst shows an ultra-low HER overpotential of 18 mV at 10 mA cm -2 and excellent stability in 1.0 M KOH. Moreover, the anion-exchange membrane water electrolyzer reaches 500 mA cm -2 at 1.70 V. This study provides a practical strategy to synthesise high-efficiency NiFe-based HER catalysts.

CAS / MDL: 7791-20-0
研究领域: 材料科学 · 电化学
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Journal of Materials Chemistry A · 2025 · IF 9.5

Nitrogen-Induced Deep Reconstruction and Formation High-Valent Nickel Species γ-NiOOH Surface Layer on NiFealloy/NiFeN Pre-catalysts for the Efficient Water Oxidation

Gouda Helal,Zhenhang Xu,Wei Zuo,Jun Qian,Gongzhen Cheng,Pingping Zhao

Transition metal-based electrocatalysts undergo electrochemical surface reconstruction to generate metal oxy-hydroxide-based hybrids, which regard the actual active sites for the oxygen evolution reaction (OER). Many efforts have been devoted to understanding the electrochemical surface reconstruction, but there is rare research to identify the origin of improved OER performance derived from the substrate. Herein, we reported the electrochemical synthesis of an amorphous γ-NiOOH surface layer on NiFealloy/NiFeN pre-catalysts for efficient water oxidation. However, the conversion of β-NiOOH to γ-NiOOH is a thermodynamically unfavorable process, resulting in much higher applied potential to drive the reaction and subsequently catalyze OER.We identified that the NiFe-bimetallic active sites can promote the OER catalytic activity more than the Ni-monometallic active sites. Besides, nitrogen can reduce the potential required to generate γ-NiOOH OER-active sites from β-NiOOH and generate the NO3- anion, which promotes the formation of γ-NiOOH. The electrochemical analysis and in situ spectroscopic approaches, including cyclic voltammetry (CV), linear sweep voltammetry (LSV), and Raman, reveal that Ni species in NiFealloy/NiFeN are more thermodynamically favorable to form γ-NiOOH than in Nialloy/NiN and NiFeLDH. Beside the electrochemical behavior, X-ray photoelectron spectroscopy (XPS), high-resolution transmission electron microscopy (HRTEM), and bode plots further demonstrate that Fe doping and nitrogen significantly increase the electrochemically active sites. Additionally, DFT calculation results show that the electronic structure of the catalysts is modulated by Fe doping, and the surface reconstruction optimized the adsorption energy of oxygen-containing species and enhanced the OER catalytic activity. This work provides a new design for constructing transition metal-based electrocatalysts for water oxidation.

研究领域: 电化学 · 材料科学 · 催化化学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2023 · IF 22.1

Promotion effect of cobalt doping on microwave-initiated plastic deconstruction for hydrogen production over iron catalysts

Wentao Li,Kezhen Qian,Zixu Yang,Xiaoxu Ding,Wenmin Tian,Dezhen Chen

Microwave-initiated deconstruction of plastic into hydrogen and high-value carbons is an attractive upcycling technology. However, the interplay between microwave field and catalyst material and the reaction mechanism were not fully understood. In this study, Co doping Fe-Al catalysts were synthesized for hydrogen production from LDPE using microwave and conventional heating. The Fe1Co1Al2 catalyst yielded hydrogen at 61.39 mmol/g plastic under microwave, which was almost two times higher than conventional heating. Characterization indicated Co doped spinel iron catalyst under microwave rapidly transformed into the highly active FeCo alloy for plastic dehydrogenation . The microwave field was responsible for the rapid formation of FeCo, as it enhanced the charge transfer from H to Fe. The Co doping also inhibited the formation of Fe 3 C during plastic deconstruction, which changed the carbon diffusion pathway and promoted the formation of nanotubes and hydrogen production.

研究领域: 化学工程 · 材料科学 · 能源技术
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Materials Today Chemistry · 2024 · IF 6.7

Copper-doped nickel–iron metal/metal oxide electrode with improved performance by promoting synergistic effects in the oxygen evolution reaction

Xiaoyu Gong,Jiawei Ge,Jun Qi,Honghe Ding,Leijie Zhang,Peiyu Ma,Zuohuan Chen,Nian Zhang,Jilong Xu,Lijuan Zhu,Jiaxiang Lu,Guiqiang Li,Junjie Ge,Yifan Ye

Advancing the performance of NiFe catalytic systems for oxygen evolution reaction (OER) is challenging, notably upon incorporating a third transition metal to create a trimetallic configuration. This study introduces a Cu-doped NiFe electrocatalyst, synthesized via a streamlined redeposition technique. The catalyst exhibits a Tafel slope of 38 mV dec −1 and a low overpotential of 248 mV at a current density of 100 mA cm −2 , plus a 2.5-fold boost in intrinsic activity. Density Functional Theory (DFT) and spectroscopic analyses demonstrate that Cu doping refines the electronic structure, enhancing charge density around the Fermi level and multiplying active OER sites. The Cu1Fe6Ni18 catalyst features robust Cu–O and Fe–O bond interactions, enhancing charge transport and OER kinetics. Our research elucidates the synergistic effects of Cu and Fe in a trimetallic system, offering an impactful approach to elevate trimetallic catalyst performance.

CAS / MDL: 13478-00-7 31175-20-9
研究领域: 材料科学 · 电化学 · 理论计算
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JOURNAL OF CATALYSIS · 2018 · IF 6.759

On the role of water in selective hydrogenation of cinnamaldehyde to cinnamyl alcohol on PtFe catalysts

Yihu Dai,Xing Gao,Xiaofang Chu,Chunyang Jiang,Yao Yao,Zhen Guo,Chunmei Zhou,Chuan Wang,Hongming Wang,Yanhui Yang

A series of carbon nanotube (CNT)-supported bimetallic PtFe nanoparticles were synthesized and employed as catalysts for hydrogenation of cinnamaldehyde in pure water. A synergy between water and bimetallic PtFe catalysts has allowed the efficiently selective production of cinnamyl alcohol. With the aid of water, an initial reaction rate of >1200 h −1 and a high selectivity of >97%, as well as a good cycling stability, were achieved with a Pt 3 Fe/CNT catalyst under mild reaction conditions. Isotopic labeling studies and theoretic calculation results demonstrated that the water-involved hydrogen-exchange pathway occurred with a lower energy barrier, which coexisted with the pathway of direct H 2 dissociation–hydrogenation. This work also suggested that water participated in the catalytic hydrogenation reaction by serving as a hydrogen-exchange bridge.

研究领域: 催化化学 · 绿色化学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Mn-mediated efficient oxygen evolution reaction on phosphorized NiFe electrocatalyst

Guangqin Gong,Jieshu Zhou,Xiulan Guo,Ruiyan Xie,Xiangke Zeng,Min Zhang,Kangni Wen,Tianding Hu,Shaoyun Shan,Kaili Yao

The development of efficient electrocatalysts for oxygen evolution (OER) is very important for the practical application of water decomposition technology. Promoting the formation of high-oxidation-state transition metal species in a hydroxide catalyst may improve its catalytic activity in the oxygen evolution reaction, which remains difficult to achieve with current synthetic strategies. Herein, we reported the synthesis of Fe x Mn y-x nanosheets on nickel foam substrate subsequently by phosphating treatment (Fe x Mn y-x P/NF). The Mn-mediated and phosphating synergistic promoting the formation of high-oxidation-state Ni and/or Fe for improved oxygen evolution activity. In-situ Raman spectroscopy showed that the incorporation of Mn and P into the NiFe hydroxide caused a cathodic shift of the NiFe hydroxide (2 + ) to NiFeOOH (3 + δ) transition potential. Density functional theory calculations suggested that an elevated oxidation state for NiFe by Mn-mediated decreased the energy barriers of the rate-determining step (*OH → *O). As a result, an overpotential of 208 mV was achieved at a current density of 10 mA cm −2 in 1 M KOH. This work provides a new strategy and a deep insight into the construction of efficient NiFe-based water oxidation electrocatalysts.

CAS / MDL: 57-13-6 1310-73-2
研究领域: 材料科学 · 电化学
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ELECTROCHIMICA ACTA · 2024 · IF 5.5

Simmer-assisted in situ synthesis of an amorphous organometallic complex-doped NiFe catalyst with nanoflower architecture for efficient electrochemical overall water splitting

Xuan Zheng,Yijun Liu,Zehua Zou,Qingxiang Wang

Developing efficient non-precious-metal-based bifunctional electrocatalysts for overall water splitting (OWS) is of great significance from both industrial and environmental perspectives. Herein, a novel flower-like architectured nanocomposite containing amorphous NiFe-hydroxide and NiFe-thiourea coordination complex, namely NiFe(O x H y )(TU)/NF, has been in situ synthesized on nickel foam by a simple simmer-assisted synthesis method. This nanomaterial demonstrates remarkable electrocatalytic performance and long-lasting durability for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Specifically, the overpotentials required to achieve a current density of 50 mA cm −2 for HER and OER are as low as 273 and 243 mV, respectively. Moreover, the OWS electrolyzer assembled using NiFe(O x H y )(TU)/NF as both anodic and cathodic electrodes operates efficiently with an exceptionally low cell voltage of 1.47 V and 1.72 V at a current density of 10 mA cm −2 and 50 mA cm −2 , exhibiting negligible fluctuation over 55 hours. And this device can also be facilely driven by the photovoltaic cell. These excellent catalytic performances of NiFe(O x H y )(TU)/NF can be attributed to the electronic synergistic effects among multiple NiFe species like NiFe-hydroxide and NiFe-thiourea, as well as the abundant active sites induced by the nanoflower-like amorphous hierarchical structure. This study presents a practical and facile strategy for the synthesis of NiFe-based amorphous nanomaterial with robust OER and HER performances, thereby contributing to the advancement of multi-component bifunctional electrocatalysts.

CAS / MDL: 7440-06-4 12036-10-1
研究领域: 材料科学 · 电化学
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CHEMICAL ENGINEERING & TECHNOLOGY · 2016 ·Vol. 39 ·期 8 ·1445-1450 · IF 2.385

Bromination of Aromatic Compounds using Bromine in a Microreactor

Qiulin Deng,Ruwei Shen,Rong Ding,Lixiong Zhang

2,4,5-Trifluorobromobenzene is a valuable intermediate with important application in the synthesis of biologically active peptides and fluorescent reagents. A continuous-flow system has been successfully developed for the synthesis of 2,4,5-trifluorobromobenzene in a microreactor using FeBr 3 as a catalyst, which is steadily generated in situ from the reaction of Br 2 and Fe. The procedure is efficient and easy-to-handle, and 2,4,5-trifluorobromobenzene can be obtained within minutes in high yields.

研究领域: 有机化学 · 合成化学
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