Energy & Environmental Science
·
2021
·Vol. 14
·期 12
·6455-6463
·
IF 38.532
Meiqi Zhao,Haoran Liu,Hongwei Zhang,Wen Chen,Hanqin Sun,Zhenhua Wang,Biao Zhang,Lin Song,Yong Yang,Chao Ma,Yunhu Han,Wei Huang
Developing a highly efficient, easy-to-fabricate and non-noble metal electrocatalyst is vital for the oxygen reduction reaction (ORR). Herein, we fabricate a single Fe site catalyst Fe1/d-CN by developing a double-layer MOF strategy. The Fe1/d-CN catalyst shows an excellent ORR activity in the pH-universal range, especially in alkaline electrolytes with a record-level half-wave potential of 0.950 V, exceeding those of almost all the reported non-noble electrocatalysts and the commercial Pt/C catalyst (0.863 V). Besides its exceptional ORR activity in alkaline electrolytes, it also exhibits comparable ORR activity to the commercial Pt/C catalyst in acidic and neutral electrolytes. We speculate that the sources of the excellent pH-universal ORR performance can be attributed to the regulation of the electronic structure of Fe centres and the excellent electron/proton transport capability that comes from the rich defects and hierarchical porous features of the Fe1/d-CN catalyst. More excitingly, the catalyst possesses remarkable durability, and exhibits a negligible decrease after 30k accelerated durability test (ADT) cycles in pH-universal media. The flexible quasi-solid-state alkaline rechargeable Zn–air batteries with the Fe1/d-CN catalyst as the cathode show superior performance such as a high OCV of 1.50 V and peak power density of 78.0 mW cm−2. Furthermore, the flexible quasi-solid-state neutral rechargeable Zn–air batteries also exhibited remarkable performance.
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高影响因子
JOURNAL OF SEPARATION SCIENCE
·
2016
·Vol. 39
·期 10
·1884-1891
·
IF 2.741
Menghua Li,Junmin Wang,Caina Jiao,Chun Wang,Qiuhua Wu,Zhi Wang
A novel magnetic porous carbon derived from a bimetallic metal–organic framework, Zn/Co-MPC, was prepared by introducing cobalt into ZIF-8. Magnetic porous carbon that possesses magnetic properties and a large specific surface area was firstly fabricated by the direct carbonization of Zn/Co-ZIF-8. The prepared magnetic porous carbon material was characterized by scanning electron microscopy, transmission electron microscopy, powder X-ray diffraction, N 2 adsorption, and vibrating sample magnetometry. The prepared magnetic porous carbon was used as a magnetic solid-phase extraction adsorbent for the enrichment of chlorophenols from water and honey tea samples before high-performance liquid chromatography analysis. Several experimental parameters that could influence the extraction efficiency were investigated and optimized. Under the optimum conditions, good linearities ( r > 0.9957) for all calibration curves were obtained with low limits of detection, which are in the range of 0.1–0.2 ng mL −1 for all the analytes. The results showed that the prepared magnetic porous carbon had an excellent adsorption capability toward the target analytes.
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ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Xiaopeng Zhang,Lin Chen,Longzhu Li,Xiaoming Yan,Junjiang Bao,Ning Zhang,Gaohong He
The introduction of guest metal molecules into metal–organic frameworks (MOFs) is an outstanding method to prepare dual-atom catalysts (DACs) with good oxygen reduction reaction (ORR) activity. However, most of the MOF-derived dual-atom catalysts reported to date exhibit a microporous structure and, therefore, suffer from the underutilization of active sites and poor mass transfer. This study employed NH2-MIL-101 as a precursor to form defect-bearing mesoporous Fe-NC via one-step pyrolysis for adsorbing [Co(en)3]3+, followed by secondary pyrolysis to generate Fe–Co binuclear site catalysts. The mesopores of NH2-MIL-101 are beneficial to [Co(en)3]3+ introduction and can improve the mass transfer of the ORR. Furthermore, the elevated nitrogen content within the [Co(en)3]3+ complex facilitates the co-coordination of Fe and Co with nitrogen, thereby enhancing the formation of Fe–Co diatomic sites. As a result, the obtained FeCo-NC-40 catalyst showed excellent ORR performance with a half-wave potential of 0.915 V (vs RHE). In addition, the liquid-phase Zn–air battery employing FeCo-NC-40 as the cathode catalyst demonstrated a peak power density of 178.13 mW·cm–2 and achieved a discharge specific capacity of 806.13 mAh·g–1 at 10 mA·cm–2, and there was no significant decay in stability for 10 days of continuous cycling.
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PubMed
高影响因子
Journal of Energy Chemistry
·
2026
·
IF 15.6
Xue Ye,Yangzhou Xu,Peipei Zhang,Dongwang Zhu,Zhicheng Chen,Yudong Xia,Fulin Yang,Xinhua Gao,Jie Li
CO 2 hydrogenation to methanol is one of the most promising pathways for emission reduction. Unlike traditional synthesis gas (CO + H 2 ) to methanol, a major challenge is that the activation of inert CO 2 at high temperature will induce the reverse water-gas shift (RWGS) reaction to generate CO, thereby reducing the methanol yield. In this research, a novel catalyst Cu 7 Zn 3 Cr 0.3 was synthesized by the carbon microsphere-assisted sol-gel method, which remarkably achieved a maximum methanol space-time yield of 345.1 g kg cat −1 h −1 under mild conditions (200 °C, 3.0 MPa, and 21600 mL g cat −1 h −1 ). Characterizations combined with theoretical simulations show that Cr doping can affect the crystal structure of ZnO, resulting in the formation of more oxygen vacancies (O V s), and induce Cu to form a stable Cu 0 -O V -Cu + active center at the interface. This active structure efficiently enhances the adsorption and activation of CO 2 , while changing the reaction path to inhibit the production of CO. The results indicate that there is a clear linear relationship between the Cu + and O V s concentration and methanol yield, which could provide experimental references for the development of high-performance catalysts for CO 2 methanol production.
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QUIMICA NOVA
·
2026
·
IF 0.9
Sun Mingzhu,Zhao Linlin
Using waste polyethylene terephthalate (PET) as the feedstock, diisooctyl terephthalate (DOTP) was directly synthesized via alcoholysis with isooctanol (2-EH) over an environmentally friendly choline chloride-zinc acetate (the ChCl-Zn(Ac)2 catalyst)-deep eutectic solvent (DES). This approach overcame the limitations of traditional methods by offering simplicity, low cost, tunable composition, excellent environmental compatibility, and superior chemical stability. The study systematically investigated the effects of reaction temperature, catalyst dosage, molar ratio of 2-EH to PET, and reaction time on the synthesis process. Response surface methodology (RSM) was employed to optimize the process conditions, with the optimal parameters determined as follows: reaction temperature of 180 °C, catalyst dosage of 5.19%, molar ratio of 2-EH to PET of 4.89 mol mol-1, and reaction time of 87.30 min. Under these optimal conditions, PET was completely degraded, and the DOTP yield reached as high as 87.59%. The ChCl-Zn(Ac)2 catalyst exhibited stable performance, significantly enhanced both the PET degradation rate and the DOTP yield. This study provides a feasible technical solution for the efficient resource utilization of waste PET, offers a reference for developing green catalytic synthesis processes of DOTP, and expands the application potential of DES catalysts in polyester degradation.
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高影响因子
Journal of Energy Storage
·
2026
·
IF 10.7
Zixiang Wan,Weicheng Zhang,Xinzhu Li,Le Huang,Zhicong Shi,Naiguang Wang
In-situ assembly and pyrolysis axially coordinate S to first sphere of Fe in Fe/S-NC. • Axial S induces the charge asymmetry of Fe–N 4 in Fe/S-NC via electronic modulation. • Lowered d-band center via symmetry breaking optimizes ORR intermediate adsorption. • Mg-air and Zn-air batteries with the Fe/S-NC catalyst exhibit superior performance. Developing efficient electrocatalysts for the oxygen reduction reaction (ORR) is essential to boosting the practical performance of Mg-air and Zn-air batteries. However, conventional non-precious Fe-N-C catalysts, with their planar Fe–N 4 sites, exhibit overly strong adsorption toward oxygenated intermediates and thus severely limit their catalytic kinetics. In this study, we report an Fe/S-NC catalyst based on an iron phthalocyanine (FePc) framework, in which a single sulfur atom is axially coordinated directly to the iron site in the first sphere. The resulting asymmetric Fe–N 4 S 1 motif breaks geometric and electronic symmetry of the iron center and thereby accelerates ORR kinetics. Theoretical calculations reveal that electronic reconstruction induced by the axial sulfur effectively optimizes the d-band center of the iron site and weakens the binding strength toward oxygenated intermediates, thus significantly reducing the energy barrier and enhancing the adsorption-desorption thermodynamics. Benefiting from this well-defined structure, the Fe/S-NC catalyst delivers half-wave potentials of 0.88 and 0.63 V (vs. RHE) in 0.1 M KOH and 3.5 wt% NaCl, respectively, and outperforms commercial Pt/C when applied in Mg-air and Zn-air batteries. This work elucidates how electronic asymmetry boosts catalytic performance and provides theoretical guidance for designing high-performance ORR catalysts. Axially coordinated sulfur atoms induce an asymmetric charge distribution at the Fe–N 4 active sites via electronic modulation. This symmetry breaking downshifts the d-band center and refines the adsorption equilibrium of oxygenated intermediates, thereby significantly accelerating the oxygen reduction reaction (ORR) kinetics and enhancing catalyst stability in both alkaline and neutral environments. Download: Download high-res image (77KB) Download: Download full-size image
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2026
·
IF 5.4
Chenxi Wang,Yichuan Li,Mantang Liu,Haonan Zeng,Yunzhi Dang,Jianhua Ma
Zn doping and BSA stabilization synergistically optimize Prussian blue nanozymes. • Zn doping narrows PB bandgap, boosting NIR photothermal conversion to 34.2%. • OSA/CMCS Schiff-base hydrogel shows self-healing and acid-triggered BPZ release. • OC@BPZ shows multi-enzyme-like ROS scavenging and > 92% antibacterial efficacy. Skin wounds are often complicated by bacterial infection, excessive oxidative stress, and mildly acidic microenvironments, which limit the efficacy of conventional single-function dressings. Here, we developed a pH-responsive dynamic composite hydrogel (OC@BPZ) by integrating bovine serum albumin-stabilized Zn-doped Prussian blue nanozymes (BPZ) into an oxidized sodium alginate/carboxymethyl chitosan Schiff base network. At the nanozyme level, BSA-mediated stabilization suppresses PB aggregation, whereas Zn doping modulates the electronic structure of the PB framework; at the matrix level, the dynamic imine network regulates the acidity-dependent release of the optimized nanozymes. The reversible imine bonds endow the hydrogel with self-healing ability, wound-conformal adaptability, and pH-responsive degradation, enabling enhanced nanozyme release under the mildly acidic wound microenvironment. The embedded BPZ nanozymes exhibit enhanced superoxide dismutase (SOD)-, catalase (CAT)-, and peroxidase (POD)-like activities, allowing efficient reactive oxygen species (ROS) scavenging and oxidative microenvironment regulation. Meanwhile, the optimized BPZ nanozymes exhibit enhanced NIR photothermal performance and antibacterial activity. Under 808 nm irradiation, OC@BPZ achieved antibacterial rates of 92.59%, 96.92%, and 97.53% against P. aeruginosa , E. coli , and S. aureus , respectively. In pH 5.5 medium, OC@BPZ released 82.4 ± 4% of BPZ over 12 days, confirming acid-responsive delivery. This cascade design combines structural responsiveness with catalytic and antibacterial functions, integrating pH-responsive release, ROS scavenging, and bacterial inhibition within a single hydrogel platform. Overall, these results demonstrate that OC@BPZ provides a promising multifunctional platform for responsive antibacterial and antioxidant wound-dressing applications. Download: Download high-res image (211KB) Download: Download full-size image An intelligent dynamic hydrogel integrating Zn-doped Prussian blue nanozymes is developed for multimodal antibacterial and antioxidant interventions. Benefiting from acid-responsive network dissociation and Zn-modulated electronic structures, it achieves on-demand nanozyme release, enabling robust multi-enzyme ROS scavenging coupled with highly efficient NIR-photothermal and ionic synergistic bactericidal capabilities.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Run Ji,Shuang Song,Lepei Wang,Hao Guo,Xiuling Zhang,Wentao Zhang
In this study, a double-layer film system was constructed with potato starch/k-carrageenan (PC) loaded with ε-polylysine-anthocyanin (ɛPL-ACN) co-pigmentation as the inner indicator layer and chitosan/gelatin (CG) loaded with ZnO-doped carbon dots (ZnCDs) as the outer protective layer. The system was designed to realize the triple functions of long-lasting bacterial inhibition, dynamic monitoring and environmental regeneration for meat packaging. When the loading concentration of ZnCDs was adjusted to 7%, the film exhibited the highest antioxidant activity (DPPH: 75.80 ± 4.01% and ABTS: 78.09 ± 2.29%), antibacterial effect ( S. aureus inhibition rate: 95.27 ± 2.17% and E. coli inhibition rate: 92.23 ± 2.24%), mechanical strength (tensile strength: 21.44 ± 0.47 MPa and elongation at break: 20.53 ± 0.81%), and light stability (ΔE: 14.71 ± 0.71). In particular, the PC-ɛPL-ACN/CG-ZnCDs-7% film exhibits excellent pH and ammonia response, which allows for the visual determination of pork freshness by color change. In terms of freshness, it extends the shelf life of pork by 4 d at 4 °C and 12 h at 20 °C. In addition, the film color difference value (ΔE) was strongly correlated with pork pH, total volatile base nitrogen and total viable count (R 2 > 0.95), which combined with smartphone RGB analysis technology can realize real-time monitoring of pork freshness. Compared with polyethylene films, PC-ɛPL-ACN/CG-ZnCDs-7% films not only have good biodegradability, but also effectively regulate the soil microbial community structure and promote the growth of crops such as Brassica rapa L ., demonstrating significant environmental sustainability advantages.
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高影响因子
ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Tianfang Yang,Ye Chen,Miao Tian,Xupo Liu,Fengxian Zhang,Jing Zhang,Kun Wang,Shuyan Gao
ABSTRACT Heteroatom doping is considered as an effective approach that manipulates the local bonding environment to improve the electroactivity of Fe-N/C catalysts. Herein, the oxidation polymerization-pyrolysis approach is applied to fabricate the uniformly F-doped porous Fe-N/C catalysts (F-FeNC) through utilizing 4-fluoroaniline as a “self-doping” precursor with N and F elements simultaneously. The synergistic effect between ligand trapping and long-range interaction of F atoms provides high density of Fe-N x active sites. The F-FeNC catalyst demonstrates superior ORR performance in alkaline media with a positive half-wave potential ( E 1/2 ) of 0.82 V, low H 2 O 2 yield of ∼3.4% and rapid 4e − transfer process. The liquid-state Zn-air battery (ZAB) assembled with F-FeNC catalyst as air cathode delivers excellent rate capability, power density (141 mW cm −2 ), specific capacity (760 mAh g − 1 ) and long-term cycle durability over 120 h. Moreover, the as-assembled all-solid-state ZAB shows excellent cycle stability at 0°∼180° bending conditions, revealing great prospects in flexible electronic device applications. Engineering the electronic structure of active sites via F self-doping provides an insightful route for designing multi-heteroatom doped Fe-N/C catalysts.
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高影响因子
Materials Today Energy
·
2023
·
IF 9.3
Li Qiao,Xingkun Wang,Ren Xu,Canhui Zhang,Kaiyue Chen,Kecheng Tong,Huanlei Wang,Shuixing Dai,Lei Chu,Minghua Huang
It is of paramount importance to develop highly efficient and Cl − corrosion-resistant bi-functional catalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) for application in seawater-based Zn-air batteries (S-ZABs), but the process remains full of challenges. Herein, a facile and effective strategy was adopted to fabricate the N-doped carbon shell armored ‘Janus’ Co/Co 9 S 8 heterojunction catalyst (denoted as Co/Co 9 S 8 -NMC). The well-defined ‘Janus’ structure endows the catalyst with a ‘synergistic effect’ between Co and Co 9 S 8 species, which can also accelerate the electron transfer via ‘Janus’ interfaces, thus boosting ORR/OER performance. Besides, N-doped carbon shells can be considered armor for protecting the catalyst from Cl − corrosion. By virtue of these merits, the resulting Co/Co 9 S 8 -NMC catalyst exhibits excellent catalytic activity for ORR and OER in seawater electrolyte, accompanied by a half-wave potential of 0.83 V and a low overpotential of 298 mV to achieve a current density of 10 mA/cm 2 . Besides, the S-ZABs based on the Co/Co 9 S 8 -NMC catalyst deliver a high maximum power density of 162.29 mW/cm 2 and robust stability over 600 h. This work advances the development of highly efficient bi-functional catalysts for S-ZABs.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Chenxi Li,Yadan Guo,Dandan Tang,Yaoping Guo,Guanghui Wang,Hao Jiang,Jun Li
The density functional theory (DFT) not only is indispensable to calculate the electronic structure and chemical property of photocatalysts, but also provides guidance to the understanding of the mechanisms involved in photocatalysis. Herein, a novel Zn doped AgFeO 2 was successfully constructed for enhancement of Cr(VI) reduction and azophloxine decomposition under visible light irradiation. The DFT calculation was employed to set up a Zn doped AgFeO 2 model to simulate its split Zn 3 d levels shift to lower energy to optimize the band structure. With Zn doped, the AgFeO 2 exhibit enhanced reducing capacity. As expected, compared to unmodified AgFeO 2 , Zn doped AgFeO 2 can reduce and remove more than 90% of Cr(VI). Based on theoretical analysis and systematic experiments, the enhanced photocatalytic of Zn doped AgFeO 2 were arisen from superoxide radical (O 2 − ) generation and photocarrier transfer via oxygen vacancies (OVs) enrichment, and the OVs would provide coordinatively unsaturated sites for Cr(VI) adsorption. We expect this work can provide new insights into the photocatalytic utilization of AgFeO 2 .
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2020
·
IF 4.551
Niu Liu,Jun Cheng,Wen Hou,Xiao Yang,Junhu Zhou
In order to form strengthened active sites for superior CO 2 adsorption on core shell ZIF-8@ZIF-67 nanocomposites , graphene oxide (GO) with oxygen-containing functional groups was used as support to synthesize hybrid adsorbents with unsaturated Zn–N 2 –O active sites. The results of XPS O 1s and FTIR analysis revealed that the Me–O functional group content in the 0.5 wt% graphene oxide (GO)-supported core shell ZIF-8@ZIF-67 nanocomposite (38.9 at.%) was much higher than that in the 0.5 wt% reduced graphene oxide (RGO)-supported nanocomposite (19.4 at.%). This was because hydroxyl functional groups in the GO formed coordination bonds with zinc atoms in core shell ZIF-8@ZIF-67. XPS N 1s spectra indicated that the incorporation of oxygen-containing functional groups in GO resulted in the transition of binding form from Me–N 4 to Me–N 2 . The CO 2 adsorption capacity of GO-supported core shell ZIF-8@ZIF-67 gradually decreased from 2.15 to 1.30 mmol/g as GO weight percentage increased from 0.5 to 4 wt%, which was consistent with the decrease in BET surface area from 1378 to 585 m 2 /g and increase in peak pore diameter from 7.7 to 8.2 Å. Density functional theory (DFT) calculations demonstrated that unsaturated Zn–N 2 –O active sites in GO-supported core shell ZIF-8@ZIF-67 nanocomposites resulted in a decreased O C⋯Zn interaction distance from 4.65 (Zn–N 4 sites in core shell ZIF-8@ZIF-67) to 3.46 Å and an increased binding energy from 34.02 to 38.87 kJ/mol. Therefore, 0.5 wt% GO-supported core shell ZIF-8@ZIF-67 nanocomposites exhibited the highest CO 2 adsorption capacity of 2.15 mmol/g (at 273 K and 1 bar), 1.34 times higher than that of core-shell ZIF-8@ZIF-67.
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危险品化学品经营许可证（带存储）