JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY
·
2021
·Vol. 21
·期 12
·6126-6134
·
IF 0
Chi Lili,Zhang Yuetong,Hua Yusheng,Xu Qiqi,Lv Mingzhu,Wang Huan,Xie Jiani,Yang Shengtao,Yong Yuan
Nanomaterials with intrinsic enzyme-mimicking characteristics, refered to as nanozymes, have become a hot research topic owing to their unique advantages of comparative low cost, high stability and large-scale preparation. Among them, Single-atom nanozymes (SAzymes), as novel nanozymes
with abundant atomically dispersed active sites, have caused specific attention in the development of nanozymes for their remarkable catalytic activities, maximum atomic utilization and excellent selectivity, the homogeneous catalytic sites and clear catalytic mechanisms. Herein, a novel single-atom
nanozyme based on Fe(III)-doped polydiaminopyridine nanofusiforms (Fe-PDAP SAzyme) was successfully proposed via facile oxidation polymerization strategy. With well-defined coordination structure and abundant Fe-Nx active sites similar to natural metalloproteases, the Fe-PDAP SAzyme exhibits
superior peroxidase-like activity by efficiently decomposing H2O2 for hydroxyl radical (.OH) species formation. Based on their superior peroxidase-like activity, colorimetric biosensing of H2O2 and glucose in vitro was performed by using a
typical 3,3,5,5-tetramethylbenzidine through a multienzyme biocatalytic cascade platform, exhibiting the superior specificity and sensitivity. This work not only provides a novel promising SAzyme-based biosensor but also paves an avenue for evaluating enzyme activity and broadens the application
of other nanozyme-based biosensors in the fields of biomedical diagnosis.
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STAR Protocols
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2022
·
IF 0
Xiao Wang,Wei Zhou,Hao Wu,Wei-Qiao Deng
Summary Single-atom catalysts (SACs) have promising atomic utilization efficiency and catalytic activity, but their construction with a specific coordination mode remains challenging. This protocol describes the synthesis of a coordinated Fe-SAC@COF for boosted electrocatalytic oxygen evolution reaction (OER). We also detail the steps for single iron atoms confinement and characterization of the COF and Fe-SAC@COF with X-ray diffraction and transmission electron microscopy technique. For complete details on the use and execution of this protocol, please refer to Wang et al. (2022) .
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Nanomaterials
·
2021
·Vol. 11
·期 7
·1847
·
IF 5.076
Yan Ma,Yujie Miao,Guomei Mu,Dunmin Lin,Chenggang Xu,Wen Zeng,Fengyu Xie
Great expectations have been held for the electrochemical splitting of water for producing hydrogen as a significant carbon-neutral technology aimed at solving the global energy crisis and greenhouse gas issues. However, the oxygen evolution reaction (OER) process must be energetically catalyzed over a long period at high output, leading to challenges for efficient and stable processing of electrodes for practical purposes. Here, we first prepared Fe-MOF nanosheet arrays on nickel foam via rare-earth erbium doping (Er0.4Fe-MOF/NF) and applied them as OER electrocatalysts. The Er0.4Fe-MOF/NF exhibited wonderful OER performance and could yield a 100 mA cm−2current density at an overpotential of 248 mV with outstanding long-term electrochemical durability for at least 100 h. At large current densities of 500 and 1000 mA cm−2, overpotentials of only 297 mV and 326 mV were achieved, respectively, revealing its potential in industrial applications. The enhancement was attributed to the synergistic effects of the Fe and Er sites, with Er playing a supporting role in the engineering of the electronic states of the Fe sites to endow them with enhanced OER activity. Such a strategy of engineering the OER activity of Fe-MOF via rare-earth ion doping paves a new avenue to design other MOF catalysts for industrial OER applications.Keywords:rare-earth doping;MOFs;large current;electronic structure
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高影响因子
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
·
2023
·
IF 4.6
Yuping Gai,Junbo Hu,Wei Deng,Wenshuo Xie,Xiang Li,Jingjing Zhang,Dewu Long,Shanlin Qiao,Fei Jiang
Summary. Electrochemical water decomposition as a crucial approach for the gradual growth of renewable energy has attracted extensive attention. Metal-organic frameworks (MOFs) which benefit from ultra-high specific surface area, controllable nanostructures, and excellent porosity have been widely used as high activity catalyst for the decomposition of water by electrochemical means. Herein, the composition and morphology of metal–organic framework nanoclusters with bimetallic Co/Fe-incorporated PTA/FDA nanoclusters is designed for efficient and durable OER electrocatalysts, including CoFe-BTC/PTA, CoFe-BTC/FDA, and CoFe-PTA/FDA. The crystal structure of MOF materials is composed of alternating organic hydrocarbon BTC, PTA, or FDA and inorganic metal oxide layer. Co and Fe interact as central atoms, joining BTC, PTA, or FDA ligands to form a highly symmetric MOF structure. The electronic structures and active sites of various metals are different, and the insertion of iron atoms plays a certain role in the regulation of their electronic structures. CoFe-PTA/FDA shows significant OER overpotential (1.525 V vs. RHE) reached 10 mA cm-2, with 62.85 mV dec-1 for Tafel slope and pretty conspicuous stability (72 hours of continuous testing). The DFT calculation results show coordination unsaturated metal atom is the primary active center of these electrocatalytic reaction, and the coupling effect caused by adding Fe is the key to adjust the electrocatalytic activity.
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BIOTECHNOLOGY LETTERS
·
2020
·Vol. 42
·期 3
·445-451
·
IF 1.977
Zhang Lei,Xu Danyu,Kong Deyong,Ji Min,Shan Lianbin,Zhao Yongjiao
Objectives To investigate the effect of zero-valent iron and copper (Fe/Cu) micro-electrolysis on dark fermentative hydrogen production from glucose by a mixed bacterial consortium and the possible mechanisms of increasing hydrogen yield. Results Compared to zero-valent iron and activated carbon (Fe/C) micro-electrolysis, Fe/Cu micro-electrolysis could increase hydrogen yield by 32.2%, hydrogen production potential by 27.1%, and the maximum hydrogen production rate by 62.0%. Meanwhile, the number of ferrous ions released into the liquid phase with Fe/Cu micro-electrolysis was about 27.0% greater than that released by Fe/C micro-electrolysis, because the dispersion of copper on the surface of iron could markedly improve electrochemical corrosion activity. Metabolic analysis revealed that Fe/C micro-electrolysis promoted acetate formation, which may have been responsible for the observed improvement in fermentative hydrogen production. Further investigation indicated that Fe/Cu micro-electrolysis increased the activity of hydrogenases and stimulated the expression of the [FeFe]-hydrogenase gene. Conclusion Fe/Cu micro-electrolysis is better than Fe/C micro-electrolysis or Fe corrosion alone for dark fermentative hydrogen production.
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高影响因子
CARBON
·
2022
·
IF 11.307
Fangqian Han,Liu Qian,Qianru Wu,Dong Li,Shulan Hao,Lihu Feng,Liantao Xin,Tao Yang,Jin Zhang,Maoshuai He
A SiC supported iron (Fe–SiC) catalyst was developed for chemical vapor deposition (CVD) growth of carbon nanotubes. Using CO as the carbon source, sole Fe–SiC catalyst was mostly inactive for synthesizing carbon nanotubes and only trace amount of carbon deposits was produced. In contrast, the powder Fe–SiC catalyst could be activated by pressing them onto a flat SiO 2 substrate or by mixing them with porous MgO powders. Particularly, efficient growth of single-walled carbon nanotubes (SWNTs) was achieved on porous MgO promoted Fe–SiC catalyst, and predominant synthesis of (6, 5) SWNTs was realized at a reaction temperature of 650 °C. Systematic characterizations revealed that the reducibility of the Fe–SiC catalyst was enhanced by the physical contact with oxide support, which promotes the formation of small active Fe nanoparticles for the subsequent SWNT nucleation and growth. This work not only deepens our understandings to the catalyst activation mechanisms, but also helps design composite catalyst for synthesizing SWNTs.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Suding Yan,Xinping Zhang,Yue Shi,Hui Zhang
The natural Fe-bearing manganese ore (FMO) and bioelectricity supplied by a single-chamber microbial fuel cell (MFC) were employed to construct the peroxymonosulfate (PMS) activation system (FMO/MFC/PMS) for the degradation of bisphenol A (BPA). The FMO was characterized by X-ray fluorescence (XRF), X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, Brunauer-Emmett-Teller (BET), field-emission scanning electron microscopy (FESEM) and transmission electron microscopy (TEM). The results show that ε-MnO 2 and α-Fe 2 O 3 were the active components of the natural FMO and they could greatly facilitate the bioelectro-activation of PMS for the oxidation of BPA. When FMO dosage, PMS concentration and current density were set as 0.5 g L −1 , 10 mM and 100 mA m −2 , respectively, 97.8% of BPA degradation could be achieved at natural pH of BPA solution after 80 min reaction and about 80% of TOC could be removed when the reaction time was prolonged to 120 min. Based on the electron paramagnetic resonance result, scavenging tests, fluorescence spectra experiment and X-ray photoelectron spectroscopy analysis, both radical oxidation (sulfate and hydroxyl radical) and non-radical reactions (such as singlet oxygen and direct electron transfer) were considered to be responsible for BPA removal. The FMO exhibited good stability and could be recycled at least 3 runs without any additional special treatment. 10 mM of Cl − and HCO 3 − could suppress the degradation of BPA while 10 mM of NO 3 − showed negligible effects on BPA removal. The FMO/MFC/PMS process could be applied in natural water without the decrease of BPA removal.
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APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING
·
2025
·Vol. 131
·期 6
·504
·
IF 2.8
Zheng Xiuxin,Gong Lin,Zou Zhengguang,Xie Zhuojia
In this paper, La 0.7 Sr 0.15 Ca 0.15 Mn 0.95 A 0.05 O 3 (A = Fe, Co and Ni) were fabricated via the sol–gel (S-G) approach. The samples are all rhombohedral structure shapes and belong to the trigonal space group R-3c, as shown by XRD. ZEISS Gemini SEM 300 scans showed irregular sub-micron particles with decreasing particle size for La 0.7 Sr 0.15 Ca 0.15 Mn 0.95 A 0.05 O 3 (A = Fe, Co and Ni). The magnetic properties were characterized utilizing an MPMS, and the magnetocaloric effects (MCE) were further investigated. The investigations of La 0.7 Sr 0.15 Ca 0.15 Mn 0.95 A 0.05 O 3 (A = Fe, Co and Ni) found that their Curie temperatures (Tc) were 289.5 K, 290.2 K, and 300 K, respectively. The maximum magnetic entropy change ( \(-\Delta {S}_{M}^{max}\) ) for La 0.7 Sr 0.15 Ca 0.15 Mn 0.95 A 0.05 O 3 (A = Fe, Co and Ni) at 5 T is 5.107 J/(kg∙K), 4.177 J/(kg∙K) and 3.852 J/(kg∙K), and the relative cooling power ( RCP ) is 264.819 J/kg, 275.3409 J/kg and 288.7435 J/kg. The Arrott curve, normalization and Curie–Weiss law (CW) fit together to determine that the second-order ferromagnetic-to-paramagnetic (FM-to-PM) transition is observed in the three samples, along with a small magnetic hysteresis and thermal hysteresis, the super-exchange interactions (SE) and the double-exchange interactions (DE) competed with each other to increase half peak width and RCP , with La 0.7 Sr 0.15 Ca 0.15 Mn 0.95 A 0.05 O 3 (A = Ni) having the largest RCP . While conventional low-temperature magnetic materials need to work in a liquid helium environment, room-temperature magnetic materials do not need to rely on extreme cooling conditions, which greatly reduces the cost of refrigeration equipment, and thus room-temperature magnetically cooled materials have a greater potential for research and development. In this paper, Ni is used as the doping element, and its RCP can reach 288.7435 J/kg, and its Tc is close to room temperature, so it is possible to be used as a room-temperature magnetic cooling material.
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高影响因子
Sustainable Energy & Fuels
·
2025
·
IF 4.1
Kexiang Li,Fancang Meng,Jiahao Li,Huan Wu,Hongbing Jia,Qingmin Ji
Polypyrrole (PPy) serves as an excellent N-rich precursor for Fe-N-C electrocatalysts, as its pyrrolic-N moieties not only facilitate metal coordination but also generate intrinsic carbon defects, promoting the formation of atomically dispersed active sites. However, excessive interchain cross-linking during polymerization often leads to dense, poorly porous carbon structures upon pyrolysis, severely limiting the accessibility of these active sites and overall catalytic performance. Herein, we report a “dynamic coordination motif” strategy by introducing 4-vinylpyridine (vP) as a co-monomer during the Fe-coordinated pyrrole polymerization. vP may compete with pyrrole for Fe coordination, forming dynamic Fe-vP complexes that act as molecular spacers within the growing polymer network. This process effectively inhibited dense chain packing, creates additional coordination anchors for Fe, and guides the formation of a more open architecture. After pyrolysis, this hybrid polymer transforms into a stable porous carbon matrix with rich pyridinic-N and a high density of accessible Fe-N sites. The resultant vP-Fe@PPy catalysts exhibited significantly superior ORR catalytic performance, outperforming both the vP-free, Fe-doped PPy-derived carbon and the commercial Pt/C catalyst. This work presents a facile and effective strategy for engineering highly accessible active sites in metal-doped carbon electrocatalysts, enabling tailorable metal loadings with uniform distribution.
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高影响因子
FUEL
·
2025
·
IF 7.5
Xiaohui Wang,Zhilong Cheng,Bingrong Liu,Huiyi Liu,Xin Fang,Ruiqi Chai,Lishuang Ma,Yuchao Lyu,Jianye Fu,Xinmei Liu
Methane dehydroaromatization (MDA) was a promising technology for the synthesis of high value-added aromatics through natural gas. Fe/ZSM-5 catalysts were widely used in MDA reaction. However, its catalytic mechanism remained ambiguous. In this work, a novel one-pot strategy was developed for the preparation of Fe/ZSM-5 catalysts, which can delicately control the iron species and acidic property of Fe/ZSM-5 catalysts. In-situ DRIFTS and DFT calculation demonstrated that MDA followed a bifunctional mechanism and the second C–H bond breaking process of CH 4 was the rate-determining step, where methane underwent coupling and dehydrogenation at the iron active sites to generate intermediate species (ethylene), and Brønsted acid sites played a key role in determining the selectivity of aromatics. Moreover, CO-pulse chemisorption revealed the quantitative synergistic effect between metal active sites and Brønsted acid sites. Catalysts with highly dispersed iron oxide and proper density of Brønsted acid sites exhibited the best catalytic performance. This study elucidated the catalytic roles of iron species and Brønsted acid sites in Fe/ZSM-5 catalysts in MDA and provided guidance for the future development of highly active MDA catalysts.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Wentao Qu,Zhikun Wang,Jiaqi Feng,Xupeng Li,Liqiang Yang,Li Wang,Jie Guo,Huiling Su,Miantuo Li,Yu Fu,Songqing Hu
This work presents a dual-adsorbent strategy for enhanced phosphate removal via chitosan-based materials with molecular-level mechanistic elucidation. Two complementary adsorbents are designed: spherical bimetallic beads (CSQ@Zr/Fe) and a porous hydrogel (CSQ@Zr). The CSQ@Zr/Fe beads demonstrate outstanding cyclic stability, retaining 84.2 % adsorption capacity after 5 regeneration cycles, while achieving a maximum adsorption capacity of 122.51 mg/g under optimized conditions. The CSQ@Zr hydrogel exhibits superior single-cycle performance with a capacity of 126.50 mg/g and rapid uptake kinetics, reaching adsorption equilibrium within 240 min. Both materials maintain high removal efficiency over a broad pH range (3–9) and show remarkable selectivity in complex ionic environments, with phosphate removal exceeding 90 % even in the presence of competing anions (Cl − , NO 3 − , SO 4 2− ). Comprehensive characterization and simulation studies reveal a synergistic adsorption mechanism dominated by electrostatic interactions (85–92 % contribution to binding energy), complemented by outer-sphere coordination (P–O–Zr: 2.25 Å; P–O–Fe: 1.85 Å) and hydrogen bonding networks. The hydrogel exhibits stronger phosphate confinement (diffusion coefficient: 0.544 × 10 −12 m 2 /s) compared to the beads (0.685 × 10 −12 m 2 /s), which correlates with its enhanced adsorption performance. This work provides not only high-performance adsorbents but also fundamental insights into the design of chitosan-based materials for sustainable phosphate removal and recovery applications.
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高影响因子
Journal of Materials Chemistry A
·
2025
·
IF 9.5
Yefei Wang,Fei Chang
The development of supported metal hydride catalysts with abundant active sites is a highly desirable yet challenging endeavor in ammonia synthesis. In this work, a lithium hydride (LiH)-loaded Fe/N-co-doped porous carbon (Fe-N-C) composite (LiH/Fe-N-C) was synthesized and demonstrated as an efficient catalyst for ammonia synthesis under mild conditions. The deposition of LiH onto Fe-N-C induced a partial reduction of the Fe-N moiety, resulting in the slight aggregation of isolated Fe single-atom sites into nanoparticles. Under reducing conditions (in the presence of H2), the coordinated nitrogen in Fe-N-C can be removed, forming nitrogen vacancies (VN), while surface iron hydride species (Fe-H) are generated through the interaction between LiH and Fe-N-C. The presence of Fe atoms adjacent to VN facilitates the adsorption and activation of dinitrogen, a process that is further supported by the replenishment of VN under reaction conditions. Notably, no lithium imide or amide species (Li2NH or LiNH2) — typically regarded as key intermediates in LiH-mediated ammonia synthesis, were observed on LiH/Fe-N-C, likely due to the fast hydrogenation step. Consequently, LiH/Fe-N-C achieves an ammonia production rate of 872 mmol·gFe-1·h-1, surpassing the performance of state-of-the-art Fe-based catalysts at 300 oC and 1 MPa. This study demonstrates that the synergistic catalysis of LiH, transition metals, and their adjacent nitrogen vacancies offers a promising pathway for efficient ammonia synthesis under mild conditions.
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