APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Xin Xiao,Yan Wei,Shaowei Song,Brian McElhenny,Fanghao Zhang,Xingxing Jiang,Yang Zhang,Shuo Chen,Mingkui Wang,Yan Shen,Zhifeng Ren
Exploiting highly efficient oxygen-evolving electrocatalysts is crucial for hydrogen production through seawater electrolysis. Here, a hierarchical structure of boron-doped (Ni,Fe)OOH grown on Ni 3 N nanosheets supported on nickel foam [denoted as B-(Ni,Fe)OOH/Ni 3 N/NF] is fabricated. Benefiting from the formation of abundant active sites and the reduced free energy barrier of the rate-determining step caused by B doping, the obtained B-(Ni,Fe)OOH/Ni 3 N/NF exhibits extraordinary electrocatalytic activity for oxygen evolution reaction, requiring overpotentials of only 283 mV and 309 mV to achieve a current density of 1000 mA cm −2 in alkaline pure water and seawater media, respectively, as well as superior stability. When driven by a commercial Si solar cell, the electrolyzer using B-(Ni,Fe)OOH/Ni 3 N/NF as the anode and a previously reported Ru/(Fe,Ni)(OH) 2 /NF as the cathode can achieve a high current of over 1000 mA in alkaline seawater media. This shows the great potential in applying a photovoltaic-driven electrolyzer toward large-scale hydrogen production in seawater electrolysis.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Xianshu Qiao,Hongjun Kang,Yang Li,Kai Cui,Xin Jia,Xiaohong Wu,Wei Qin
Developing the high-performance intermetallic bi–metal boride OER catalysts with a high density of grain boundaries and appropriate electronic structure is still a challenge. Herein, we synthesized an intermetallic (Fe x Co 1− x ) 2 B OER catalyst (GB-(Fe x Co 1− x ) 2 B) with controllable grain boundary densities by a facile ball-milling method. Benefiting from the modulation of both grain boundary density and electronic structure, the GB-(Fe 0.66 Co 0.34 ) 2 B supported on reduced graphene oxide shows a low OER overpotential of 221 mV at a current density of 10 mA cm −2 and Tafel slope of 38.2 mV dec −1 . The experimental and theoretical calculated methods demonstrate that the Fe introduction into the intermetallic Co 2 B catalyst can produce the higher grain boundary density and modulate the electronic structure, respectively. This work provides a promising insight in understanding the synergetic effects in bimetallic for GB-(Fe x Co 1− x ) 2 B systems and supports a new strategy to explore other efficient catalysts with a high density of grain boundaries.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Qingtao Liu,Weihao Liu,Xin Wan,Weiwei Chen,Xiaozhi Liu,Xiaofang Liu,Jiaxiang Shang,Jungang Miao,Dong Su,Xin Sun,Jianglan Shui
Zeolitic imidazolate framework-8 (ZIF-8) is widely used as precursor for carbon-supported single-metal-atom catalysts (M–N–C), but typically yields amorphous carbon with poor stability in proton-exchange-membrane fuel cells (PEMFCs). Traditional methods would lose active site density while increasing the graphitization degree. Here, this study reports that ultra-small nano ZIF-8 can produce graphene-nanostacks-based Fe–N–C that has improvements on both activity and stability. First, anti-sintering nanoporous ZIF-8 (nano-ZIF8) particles are synthesized with unit size of 8 nm (the smallest so far) using a destruction-reconstruction strategy. In situ microscopy reveals that the volatilization of Zn has a decisive effect on the graphitization degree of ZIF-8 and such process is size-dependent. Nano-ZIF8 particles have completed Zn volatilization before graphitization process beginning, leading to graphene nanostacks. These nanostacks preferentially host edge-type FeN 4 sites, which have doubled intrinsic activity and much improved stability compared with conventional Fe−N−C. In PEMFC, the catalyst achieves an activity of 48.5 mA cm − 2 @0.9V iR -free , meeting the US Department of Energy 2025 activity target. In addition, quantitative analysis of active site density is conducted in PEMFC for the first time using nitrite stripping voltammetry. The unique graphitization behavior of nano-ZIF8 paves a new avenue for advancing M–N–C catalysts.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Jie Liu,Xinru Wei,Shan Lu,Ningyuan Song,Yanru Liu,Shu Yang,Fangxu Dai,Yunmei Du,Lei Wang
How to skillfully enhance the OH - binding energy of the hydrophilic site to accelerate water decomposition and avoid OH - poisoning is a huge challenge for achieving efficient alkaline HER kinetics. Therefore, the Ru-Fe 2 P/Re 3 P 4 model was designed from the perspective of coordinating the binding energy and spillover path of OH - . Density functional theory (DFT) disclosed that Re and Ru atoms act as hydrophilic sites and hydrogen evolution sites, respectively, to synergistically promote alkaline HER. In addition, the Ru dopant reduced the water dissociation energy barrier by enhancing the OH - binding energy of the Re hydrophilic sites. Meanwhile, Fe atoms with stronger OH - binding energy exhibited the OH - detoxification effect by promoting the OH - dynamic spillover from the Re sites. Given these, a unique Ru-ReFeP/IF-Q electrode was prepared by the ‘vapor phase phosphorization-quenching Ru doping’ strategy. As anticipated, the Ru-ReFeP/IF-Q electrode, driven by the Re-Ru-Fe alkaline hydrogen evolution reaction (HER) mechanism, only requires an overpotential of 172 mV at the industrial-level current density of 1 A cm −2 . The reinforced signal peaks attributed to Ru-H and Fe-OH species in the in-situ Raman spectra confirmed the detoxifying effect of Fe sites in avoiding OH - poisoning at hydrophilic active sites. In summary, this work provides a novel design idea for accelerating alkaline HER kinetics from the perspective of synergistically optimizing the binding energy and spillover path of OH - byproducts.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Zhanqin Wang,Fei Shao,Mingzhe Dong,Xingwu Zou,Bo Li,Yan Jing,Shuxuan Wang,Yongzhong Jia
The rational design of high-performance adsorbents for lithium recovery from aqueous resources depends critically on understanding how metal doping modulates the structure and properties of metal-organic frameworks (MOFs). In this work, we systematically investigate the effects of Fe doping on the lithium adsorption and isotope separation performance of Al-MOFs through controlled synthesis of bimetallic Al/Fe-MOFs with varying metal ratios (1:4 to 4:1). The materials were characterized by XRD, XPS, TGA, and adsorption experiments, complemented by density functional theory calculations. Results show that optimal Fe incorporation (Al/Fe = 2:1) significantly improves Li + adsorption capacity (24.07 mg g −1 ) and isotopic selectivity ( α = 1.033) compared to the undoped MOFs ( Q = 12.97 mg g −1 , α = 1.027). Structural analyses reveal Al/Fe-MOFs contraction (Δ d (002) = 0.36 Å) and surface charge modification (pH ZPC shift from 10.26 to 8.73), while electronic structure studies demonstrate Fe 3+ /Fe 2+ redox activity promotes electron transfer. DFT calculations identify greatly increased adsorption energetics (−3.96 eV) through synergistic Al O/Fe O interactions, where the rigid Al O framework ensures structural stability and flexible Fe O sites support dynamic adsorption. The material exhibits excellent cycling stability (92 % capacity retention) due to dual stabilization mechanisms. These findings confirm that balanced bimetallic coordination in MOFs can enhance adsorption capacity and selectivity through geometric and electronic effects, providing valuable insights for designing advanced adsorbents for lithium recovery.
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高影响因子
APPLIED ENERGY
·
2025
·
IF 11
Xianda Sun,Baibin Ma,Jinxu Hao,Zirui Wu,Yi Li,Hao Liu,Yuandong Yang,Xiaohan Ren
The ammonia crossover that poisons the conventional cathode catalysts and damages the cell performance and efficiency is one of the paramount bottlenecks limiting the development of direct ammonia fuel cells (DAFCs). Synthetizing the ammonia tolerance catalysts has been proven to be an effective avenue to solve the above-mentioned problems, however, the mass and charge transports within the anti-ammonia poisoning electrodes has not been fully elucidated. Herein, an alkaline DAFC with anti-ammonia poisoning Fe-N-C cathode is reported, and the main effort is expended on investigating the impact of mass and charge transports on cell performance, internal resistance, and operating stability. The alkaline DAFC exhibits a thermodynamic efficiency as high as 88.6 %, higher than that of hydrogen-based fuel cells. The preliminary experimental results indicate that the performance of DAFC with anti-ammonia poisoning Fe-N-C cathode is higher than that of conventional Pt/C cathode under the same catalyst loading. The impressive open-circuit voltage of 0.74 V and peak power density of 107 mW cm −2 are obtained under atmospheric pressure and 80 °C, which is primarily ascribed to both the anti-ammonia poisoning of Fe-N-C catalyst and the facilitated mass and charge transports. Furthermore, the voltage curve of DAFC is quite stable during the constant-current discharging at 100 mA cm −2 for 10-h, demonstrating the good durability of DAFC with anti-ammonia poisoning Fe-N-C cathode.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Mian Li,Lian-Yu Qiu,Tian-Yang Zhang,Bin Xu,Dan Yang,Ting Ye,Heng Luo
Advanced oxidation processes (AOPs) based on Fe 2+ /persulfate (PS) have been widely applied in water treatment but face critical challenges: inefficient radical utilization due to excess Fe 2+ scavenging, unsustainable reactivity from irreversible Fe 2+ -to-Fe 3+ conversion, and ambiguous dominant reactive species (e.g., SO 4 − / OH vs. high-valent iron). Ferric oxalate complexes address these limitations by enabling light-driven iron photoreduction and the Fe 2+ /Fe 3+ cycle. However, direct comparisons of degradation efficiency, mechanisms, and environmental risks between Fe 2+ /PS and UV/Fe(C 2 O 4 ) 3 3− /PS remain scarce. Using iohexol as a model, this study directly compared the two systems. The UV/Fe(C 2 O 4 ) 3 3− /PS system achieved 98.8 % iohexol degradation in 60 min (vs. 69.9 % for Fe 2+ /PS) and reduced iron sludge by 70–80 %. Both systems relied on SO 4 − and OH, but UV/Fe(C 2 O 4 ) 3 3− /PS enhanced radical yield via photocatalytic iron cycling, whereas Fe 2+ /PS depended on Fe(IV). In Fe 2+ /PS, contributions were Fe(IV) (29.4 %) > SO 4 − (25.9 %) > OH (20.2 %); in UV/Fe(C 2 O 4 ) 3 3− /PS, SO 4 − (63.6 %) > OH (23.7 %) > Fe(IV) (23.7 %). Electrical energy per order (EE/O) analysis showed UV/Fe(C 2 O 4 ) 3 3− /PS consumed 1.166 kWh mM −1 , 60.2 % lower than Fe 2+ /PS (2.524 kWh mM −1 ). Acute toxicity tests with Vibrio fischeri exhibited 67.7 % inhibition in Fe 2+ /PS, significantly higher than 36.4 % in UV/Fe(C 2 O 4 ) 3 3− /PS. Ecological Structure-Activity Relationships (ECOSAR) modeling and disinfection by-products (DBPs) risk assessment further confirmed lower risks in UV/Fe(C 2 O 4 ) 3 3− /PS, with 50 % lethal concentration ((LC 50 ) for aquatic organisms 2.3-fold higher and genotoxicity potency 41.7 % lower than Fe 2+ /PS. These results bridge the efficiency-risk gap between the two systems and offer a three-dimensional (efficiency-cost-safety) framework for AOP selection.
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高影响因子
Science Advances
·
2022
·Vol. 8
·期 40
·
IF 14.957
Jingzhong Qin,Bo Han,Xixi Liu,Wen Dai,Yanxin Wang,Huihui Luo,Xiaomei Lu,Jiabao Nie,Chensheng Xian,Zehui Zhang
The cleavage and functionalization of recalcitrant carbon─carbon bonds is highly challenging but represents a very powerful tool for value-added transformation of feedstock chemicals. Here, an enzyme-mimic iron single-atom catalyst (SAC) bearing iron (III) nitride (FeN 3 ) motifs was prepared and found to be robust for cleavage and cyanation of carbon–carbon bonds in secondary alcohols and ketones. High nitrile yields are obtained with a wide variety of functional groups. The prepared FeN 3 -SAC exhibits high enzyme-like activity and is capable of generating a dioxygen-to-superoxide radical at room temperature, while the commonly reported FeN 4 -SAC bearing FeN 4 motifs was inactive. Density functional theory (DFT) calculation reveals that the activation energy of dioxygen activation and the activation energy of the rate-determining step of nitrile formation are lower over FeN 3 -SAC than FeN 4 -SAC. In addition, DFT calculation also explains the catalyst’s high selectivity for nitriles.
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高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2015
·Vol. 17
·期 40
·26690-26702
·
IF 4.493
Shengjie Xia,Mengmeng Shao,Xiaobo Zhou,Guoxiang Pan,Zheming Ni
A series of novel organic–inorganic nanoscale layered materials were synthesized by intercalating the Ti-containing Schiff base complex into the interlayer of the ZnM layered double hydroxides (LDHs, M = Al, Cr, Fe, Ce). The hybrid material was further calcined to make metal oxide composites with highly dispersed Ti elements (Ti/ZnO–MxOy). The structural characterization and photocatalytic results showed that, after intercalation and calcination, the metal oxide composites with a unique flower-like crystal morphology not only had high specific surface area, uniform pore size distribution and narrow band gap, but also showed extremely high photocatalytic performance for hexachlorobenzene (HCB) degradation. The Ti/ZnO–Cr2O3 composite with the narrowest band gap (2.40 eV) and the highest surface area (227 m2) showed the highest photocatalytic performance for HCB (95.5% within 240 min) among the four metal oxide composites. Particularly, it was found that composites derived from layered materials with different supramolecular structure of the host and guest showed different photocatalytic properties. In addition, based on the results from ESR, GC-MS and HPLC-MS, the type and amount of hydroxyl radicals, the decomposition intermediates and the pathway of HCB degradation photocatalyzed by Ti/ZnO–MxOy composites are also discussed in detail.
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高影响因子
Materials Chemistry Frontiers
·
2017
·Vol. 1
·期 10
·2065-2077
·
IF 0
Fu Yang,Bangbang Wang,Hang Su,Shijian Zhou,Yan Kong
Surface defective or heterojunction sites of catalysts generally afford remarkable catalytic activity thanks to their high-surface-energy. Regularly-generating multiple defective sites on the surface of a catalyst is exceedingly promising in many reactions. In this study, we report an unexpected Co/Fe–Co planar hybrid composite nanosheet with serried surface defects including surface biphasic junction sites or defective holes. A facile thermal-induced process was applied to trigger the generation of defective sites on planar Co/Fe–Co hydroxides. Through a controlled thermal process, massive serried CoO nanocrystals were in situ dissolved out of the surface of cobalt hydroxide, while defective surface holes were formed on the Fe-doped Co(OH)2 nanosheets under a prolonged thermal procedure. The morphology and microscale structure of the resulting Co/Fe–Co hybrid 2-dimensional (2D) composites were systematically examined by virtue of various characterization techniques. As expected, the obtained surface defective Co/Fe–Co planar composites showed obviously enhanced catalytic activity in the Fenton-like reaction. Based on a catalytic study, we proved that the CoO nanocrystals densely-distributed on thinlayer Co(OH)2. Uniformly-introduced Fe heteroatoms in the inter-structure of Co(OH)2, along with the formed surface defective holes on Fe–Co hybrid composites, are synergistically responsible for increased catalytic removal efficiency of MB in the presence of peroxomonosulfate.
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ANALYTICA CHIMICA ACTA
·
2021
·
IF 6.558
Jiabi Xu,Yanyan Xing,Yutong Liu,Mingzhe Liu,Xiaohong Hou
In recent decades, artificial nanozymes with excellent stability, low cost and availability have been gradually explored to avoid the limits of natural enzymes such as poor stability, high cost and difficult preparation. Herein, for the first time, we investigated the capability of nanoscale Fe 3 O 4 @MIL-100(Fe) as a nanozyme, which was quickly synthesized in situ by a microwave-assisted method within 20 min using Fe 3 O 4 as the metal precursor. The obtained Fe 3 O 4 @MIL-100(Fe) showed satisfactory intrinsic dual enzyme mimetic activities, including peroxidase (POD)- and catalase (CAT)-like activities. Moreover, a simple and effective colorimetric biosensor was fabricated to detect glutathione (GSH) based on its POD-like activity. The proposed measurement had a linear range of 1–45 μM and a limit of detection (LOD) of 0.26 μM (3.3 δ/S). It was proved that the established colorimetric sensing system could be successfully applied to detect GSH in actual biological samples. Importantly, the outstanding reusability and stability made it extremely valuable as a catalyst. The present work implied that Fe 3 O 4 @MIL-100(Fe) synthesized in situ by the microwave-assisted method was a very promising candidate for biocatalyst and biosensing.
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高影响因子
Journal of Inorganic and Organometallic Polymers and Materials
·
2023
·Vol. 34
·期 4
·1751-1764
·
IF 4
Zhou Zhuyou,Zou Congyang,Wang Yong,Liu Menghe,Ji Yufeng
A one-step solvothermal synthesis technique was employed to fabricate C 60 /MIL-101(Fe) composites. The C 60 /MIL-101(Fe) composites showed a better performance in the degradation of methylene blue (MB) and tetracycline hydrochloride (TCH) when compared to MIL-101(Fe) in the photo-Fenton system, which can be credited to the charge transfer and separation facilitated by the addition of C 60 . Results showed that C 60 /MIL-101(Fe) had the capacity to nearly completely eliminate TCH and MB over a broad pH range. The catalysts demonstrated remarkable catalytic degradation on various organic pollutants and water samples. Through active substance quenching experiments and EPR, it was determined that hydroxyl radical (·OH) is the main factor in the photocatalytic reaction process.
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高影响因子
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