APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Cong Gao,Yan Su,Xie Quan,Virender K. Sharma,Shuo Chen,Hongtao Yu,Yaobin Zhang,Junfeng Niu
Heterogeneous Fenton-like reaction was a promising approach for generating •OH. However, the heterogeneous catalysts generally exhibited low activity because of slow reduction of Fe(III) in Fe(III)/Fe(II) redox cycle. Here, decreasing electron density was expected to quicken Fe(III) reduction and consequently enhance the catalytic activity of heterogeneous catalysts. This hypothesis was validated by the enhanced hydroxyl radicals generation and accelerated Fe(III) reduction on MIL-88B(Fe)-X (2-X-terephthalic acid, X = NH 2 , CH 3 , H, Br and NO 2 ) by reducing electron density of Fe(III) with substituent of higher electrophilicity. MIL-88B(Fe)-NO 2 , with the substituent of highest electrophilicity among these catalysts, has the lowest electron density of Fe(III) and highest redox potential ( E Fe(III)/Fe(II) = 0.35 V). As a result, it exhibited the best catalytic performance, which was 1.7–20 times higher than that for other MIL-88B(Fe)-X and was comparable to that of homogeneous Fe 2+ . This study provides scientific basis for rational construction of highly effective heterogeneous Fenton-like catalyst.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Xiaobing Wang,Chengyu Wei,Xiaosheng Song,Zuohui Wang,Yong Zhao
In the oxygen evolution reaction (OER), the non-reversible destruction of surface electronic structure caused by the irregular element migration in complex surface/interface reaction limits the improvement of catalyst’s activity and stability. Herein, we successfully realize the control of ‘dual-path migration of metallic elements in OER’ to stepwise reconstruct the O-coordinated bi-metal heterodimer (M 1 -O-M 2 ) for electron density redistribution. By designing Fe@FeNi 3 @NiO-Fe 3 O 4 (F-FN-NFO) model electrode with stepwise surface treatment in OER process, the directional migration (from core to shell, path 1 ) and adjacent-surface migration of Fe atoms ( path 2 ) are both controlled to reduce the formation energy of Ni-O-Fe units, realizing strengthened electron transfer between heterogeneous metal centers. After the surface reconstruction, the OER activity of F-FN-NFO increases for 8.6 times at 1.7 V (30.5–263 mA cm −2 ). Based on this strategy, the designed three-dimension NiFe@NiFe x O is positive activated compared to traditional NiFe-oxidation with the overpotential reduced to 299 mV at 10 mA cm −2 .
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CHEMOSPHERE
·
2023
·
IF 8.8
Chunsheng Ding,Xinze Song,Zhongyi Zheng,Hainan Wang,Yuqiang Pan,Hangtian Zhang,Xueyan Li,Jing Deng
Fe(II)-catalyzed PMS process was widely used in the degradation of refractory pollutants in wastewater, while its performance was restricted by the slow regeneration efficiency of Fe(II). Herein, caffeic acid (CFA), a representative of hydroxycinnamic acids, was introduced into Fe(III)/PMS system to accelerate the transformation of Fe(III) to Fe(II) and promote the removal of bisphenol A (BPA). Under optimum condition of 0.1 mM CFA, 0.05 mM Fe(III), and 0.5 mM PMS, almost complete removal of BPA can be achieved within 20 min, which was roughly 6.2 times higher than that in Fe(III)/PMS system. As the addition of CFA into Fe(III)/PMS system, pH application range was widened from acidic to alkaline conditions. The reduction and chelation of CFA expedited the Fe(III)/Fe(II) cycle by forming CFA-Fe chelate, thereby facilitating the PMS activation . Based on LC-MS analysis and DFT calculation, the intermediate products of CFA were found to play a decisive role in boosting the regeneration of Fe(II), and the toxicity of these intermediates towards organisms was evaluated by ECOSAR . The alcohol-scavenging and chemical probe tests certified that hydroxyl radical (•OH), sulfate radical (SO 4 •- ), and Fe(IV) coexisted in Fe(III)/CFA/PMS system, and the second-order reaction rate constants of •OH and SO 4 •- reacted with CFA were calculated to be 3.16✕10 9 and 2.30✕10 10 M −1 s −1 , respectively. Two major degradation pathways of BPA, •OH addition and SO 4 •- induced hydroxylation reaction, were proposed. This work presented a novel green phenolic compound that expedited the Fe(II)-catalyzed PMS activation process for the treatment of organic contaminants .
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Xiaoqi Zhao,Yingxiao Li,Xue Zhang,Yanfang Gao,Ling Liu
Surface oxygen vacancy increases active site numbers, and multidimensional cross-linked structure improves the exposure of active sites. Thereby, they can enhance the oxygen reduction reaction (ORR) performance of Fe-N-C catalysts effectively. Herein, Fe(NO 3 ) 3 ·9H 2 O and carbon nanotubes (CNTs) were introduced into zeolitic imidazolate framework nano leaves (ZIF-L) to prepare multidimensional cross-linked Fe-N-CNTs with surface oxygen vacancies through co-pyrolysis at the high-temperature. As expected, the synthesized multidimensional cross-linked Fe-N-CNTs-900-0.2 composite rich in oxygen vacancies increased the conduction band potential and improved the reducing capacity. Thus, Fe-N-CNTs-900-0.2 possessed a better ORR electrochemical performance (half-wave potential = 0.892 V vs. RHE) that surpass the Pt/C catalysts. Moreover, the Al-air batteries containing Fe-N-CNTs-900-0.2 displayed a higher maximum power density than those of Pt/C catalysts. The electronic band structure shows that Fe-N-CNTs-900-0.2 rich in oxygen vacancy concentration has higher conduction band potential and effectively improves the activity of ORR catalysts. This work innovatively proposes that the joint work of multidimensional cross-linked structure and oxygen defects is an effective method to enhance the ORR performance and clarifies its internal reaction mechanism, which provides a new idea to design and preparer Fe-N-C catalysts.
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MICROCHIMICA ACTA
·
2023
·Vol. 190
·期 5
·1-10
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IF 5.7
Wei Chunying,Lin Huiqing,Bai Hehe
Five G-/C-rich single-stranded DNA (ssDNA) with different sequences and lengths were templated to prepare the DNA-Cu, DNA-Fe, and bimetallic DNA-Cu/M nanoclusters (NCs). The peroxidase-like activities of these nanomaterials were studied using H 2 O 2 and 3,3′,5,5′'-tetramethylbenzidine (TMB) as the reaction substrates in HAc-NaAc buffer. It was found that T30-G2-Fe NCs and T30-G2-Cu/Fe NCs, with a size of about 2 nm, exhibit similar and the strongest enzyme-like activity under optimal conditions. Both NCs possess a similarly high affinity to substrates, and the Michaelis–Menten constant ( K m ) values to TMB and H 2 O 2 are about 11 and 2–3 times lower than those of natural horseradish peroxidase (HRP), respectively. The activity of both nanozymes decreases to about 70% after being kept for one week in pH 4.0 buffer at 4 °C, which is comparable with HRP. Hydroxyl radicals (•OH) are the main reactive oxygen species (ROS) produced in the catalytic reaction. Moreover, both NCs can facilitate in situ generation of ROS in HeLa cells using endogenous H 2 O 2 . MTT assays indicate that the T30-G2-Cu/Fe NCs exhibit the strong selective cytotoxicity to HeLa cells over HL-7702 cells. The cellular viability is about 70% and 50% after incubating with 0.6 M NCs for 24 h without or with 2 mM H 2 O 2 , respectively. The current study shows that the T30-G2-Cu/Fe NCs have the potential for chemical dynamic treatment (CDT). Graphical abstract
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2023
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IF 4.3
Yunxin Shi,Liying Wang,Xin Miao,Zhenzhu Cao,Yongfeng Zhang,Lin Cheng,Jucai Yang
A series of donut-like nanostructured heterojunction materials are first synthesized via one-step solvothermal method to improve the photocatalytic efficiency for the environmental pollutants. The unique donut-like Fe-doped-BiOCl@Fe-MOF heterojunction with uniform size guarantees suitable surface area and many active sites for the model pollutant. The optimal photocatalytic efficiency is shown in degradation of RhB (99.0 %, 90 min) and TC (90.4 %, 90 min) solution, which had higher photocatalytic efficiency than a variety of similar materials previously reported. The result revealed that the enhancing photocatalytic activity is mainly depended on the synergistic effect of Fe-MOF and Fe-doped BiOCl. The possible mechanism is further studied, which shown h + and O 2 − are the primary active species in the degradation process of RhB and TC solution. Meantime, Fe-doped BiOCl@Fe-MOF with the excellent reusability and stability. After the fourth cycle, the degradation rate of RhB solution can still be as high as 86.4 %. In this work, we provide a higher efficiency heterojunction photocatalytic material by varying the organic ligand content.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2025
·
IF 6.2
Mingqiang Chen,Quan Wang,Defang Liang,Yishuang Wang,Chang Li,Xuemei Shen,Chunyue cheng,Jun Wang
Herein, a series of Fe-based biochar catalysts (xFe/WSBC) were synthesised via impregnation using wheat straw as a carbon precursor and applied to the Fischer–Tropsch synthesis of olefins (FTO) from syngas. Various characterisations of fresh catalysts demonstrated that Fe content significantly affected the dispersion of iron particles and the surface distribution of Fe 3 + /Fe 2+ . Among the samples, 5Fe/WSBC exhibited the highest surface Fe 3+ /Fe 2+ ratio and thus the lowest surface electron density, which enhanced the adsorption and activation of H 2 . In addition, an appropriate amount of the Fe additive (5 wt%) significantly decreased the Fe 3 O 4 particle size, which promoted the continuous reduction and carbonisation processes during FTO to generate iron carbide phases, which boosted CO activation and the subsequent C–C coupling. Therefore, 5Fe/WSBC exhibited the highest CO conversion (46.9 %) and iron time yield (348.9 μmol CO ·g Fe −1 ·s −1 ) as well as the major enhancement of selectivity to light olefins (C 2 = –C 4 = ). The results for the used catalysts demonstrated that 5 wt% Fe clearly inhibited the sintering of iron particle size and improved the catalytic stability of FTO.
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ACS Nano
·
2024
·
IF 15.8
Qing Luo,Qian Ma,Taoxia Liu,Yiting Luo,Lianying Wang,Chang Guo,Leyu Wang
We developed an intrinsic hydrophilic single-atom iron nanobowl (Fe-SANB) for magnetic resonance imaging (MRI)-guided tumor microenvironment-triggered cancer therapy. Benefiting from the sufficient exposure of Fe single atoms and the intrinsic hydrophilicity of the bowl-shaped structure, the Fe-SANBs exhibited a superior performance for T1-weighted MRI with an r1 value of 11.48 mM–1 s–1, which is 3-fold higher than that of the commercial Gd-DTPA (r1 = 3.72 mM–1 s–1). After further coembedding Gd single atoms in the nanobowls, the r1 value can be greatly improved to 19.54 mM–1 s–1. In tumor microenvironment (TME), the Fe-SANBs can trigger pH-induced Fenton-like activity to generate highly toxic hydroxyl radicals for high-efficiency chemodynamic therapy (CDT). Both the MRI and CDT efficiency of these nanobowls can be optimized by tuning the ratio of Fe(II)/Fe(III) in the Fe-SANBs via controlling the calcination temperature. Furthermore, the generation of •OH at the tumor site can be accelerated via the photothermal effect of Fe-SANBs, thus promoting CDT efficacy. Both in vitro and in vivo results confirmed that our nanoplatform exhibited high T1-weighted MRI contrast, robust biocompatibility, and satisfactory tumor treatment, providing a potential nanoplatform for MRI-guided TME-triggered precise cancer therapy.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Jiaojiao Sun,Mengxia Shen,A.jun Chang,Jianfeng Huang,Pengbo Wang,Yonghao Ni
Conventional metal-nitrogen-carbon single-atom catalysts (M-N-C SACs) are plagued by electron localization effects arising from symmetric coordination geometries and the absence of synergistic interactions among isolated active sites, both of which critically undermine oxygen reduction reaction (ORR) catalytic performance. To address these limitations, this study introduces a multiscale synergistic engineering strategy that integrates asymmetric coordination design with bioinspired structural innovation. Specifically, the symmetry of the Fe-N 4 coordination is disrupted to generate Fe-N 3 Se sites, which facilitate charge density redistribution; while Fe atomic clusters (FeACs) are strategically integrated to construct asymmetric catalytic centers that activate O 2 and promote O-O bond cleavage. A hierarchical porous carbon submicronspheres architecture, inspired by alveolar structures and featuring gradient-distributed micropores and mesopores, has been developed to enhance the mass transport efficiency at triple-phase interface. Overall, we have developed FeSAs and FeACs anchored on alveolar-inspired hierarchically porous nitrogen/selenium co-doped carbon submicronspheres (Fe SA+AC -N/Se-AHCs), which exhibits outstanding ORR activity (E o =0.99 V, E 1/2 =0.90 V) and long-term durability. Theoretical analyses further demonstrate that the electronic coupling between Fe-N 3 Se sites and FeAC synergistically optimizes the adsorption free energies of critical *OOH and *O intermediates, thereby accelerating O-O bond dissociation. This work presents a comprehensive cathode catalyst platform for developing high-energy-density and long-cycle-life Zinc-air batteries.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 42
·20490-20496
·
IF 3.925
Ling Li,Jing Wu,Lieyuan Huang,Gaoli Lan,Naxiang Wang,Hui Zhang,Xin Chen,Xingbo Ge
Commercial applications of electrolytic water splitting require cost-efficient and active oxygen evolution catalysts. Nickel–iron (NiFe)-based compounds have attracted significant attention as oxygen evolution reaction (OER) catalysts due to their high catalytic activity. We develop a simple and easily controlled method by combining anodic fluoridation and cyclic voltammetry (CV) treatment to convert NiFe alloy to Ni/Fe hydroxide. A cracked layer structure of Ni/Fe hydroxide formed on the surface during the fluoridation of NiFe alloy and the CV process in KOH. The Ni/Fe hydroxide exhibits considerable OER activity with an onset potential of 1.47 V vs. RHE and a Tafel slope of 47 mV dec−1 in 0.1 M KOH. The electrode also shows an acceptable stability in alkaline media. The results indicate that anodic fluoridation and CV treatment are promising methods to form active layer structures of hydroxide on transition metals and their alloys, further increasing the electrocatalytic activity of the catalyst.
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Journal of Water Process Engineering
·
2025
·
IF 6.7
Jiangfu Zheng,Xiaoming Li,Jinglin Ding,Xingong Li
Research on peroxymonosulfate (PMS) activation via catalytic processes for degrading trace organic pollutants in aquatic environments has attracted considerable interest. Although iron is widely used in homogeneous advanced oxidation processes (AOPs), its effectiveness in activating PMS remains suboptimal. This study demonstrates that the environmentally benign chelating agent ethylenediamine- N , N ′-dibutyldicarboxylate (EDDS) markedly enhances iron-mediated PMS activation. With six coordination sites, EDDS forms stable five- and six-membered chelate rings with Fe(III)/Fe(II) ions, facilitating efficient PMS activation and leading to complete degradation of NTP. Beyond improving iron's catalytic performance, EDDS also inhibits iron disproportionation, thereby promoting PMS activation and facilitating NTP mineralization. Moreover, the system achieved removal efficiencies exceeding 96 % for tetracycline (TC), ciprofloxacin (CIP), sulfamethoxazole (SMX), and methylene blue (MB) within 35 min. Systematic experiments elucidated the critical role of the Fe(III)/Fe(II) redox cycle in the HeLDH/EDDS/PMS system, highlighting the central involvement of Fe(III) species in the regeneration of Fe(II). Multiple reactive oxygen species, including •OH, SO₄• − , RO•, O₂• − , and 1 O₂, were identified as contributors to NTP degradation. Transformation pathways and mechanistic details of NTP degradation were revealed via mass spectrometry, and toxicity evaluations confirmed a significant reduction in the ecotoxicity of oxidation products. The system also exhibited strong resistance to humic acid interference and effectively degraded multiple organic contaminants, underscoring its potential for sustainable water purification applications.
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NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Lei Dong,Yangyang Yuan,Shengjie Zhu,Peidong Li,Xiaomin Zhang,Yanping Chen,Lei Xu
Direct synthesis of dimethyl carbonate (DMC) using CO2 and methanol as raw materials is an environmentally friendly and promising route for recycling carbon sources from exhaust gases. Herein, well-constructed CeO2-based nanoparticle catalysts promoted by various Fe contents were synthesized via a facile co-precipitation method and demonstrated to be highly effective for direct DMC synthesis. The uniform doping of iron species in ceria lattice resulted in the formation of more surface oxygen vacancies, and thereby more coordinatively unsaturated surface metal cations and lattice oxygen anions were generated, which served as the Lewis acidic-basic sites required for the reaction. Based on in-situ DRIFTS results, it was deduced that the oxygen vacancies played a crucial role in activating CO2 to reactive bidentate carbonates and the formation of active terminal methoxy intermediates was also enhanced by Fe incorporation. Consequently, the maximum DMC yield of 3.84 mmol h-1 g-1 cat was obtained on Fe0.04Ce0.96Ox under relatively mild reaction conditions of 130 °C and 3.0 MPa. Additionally, in the tandem reaction system using 2-cyanopyridine (2-CP) as a dehydrating agent, the catalytic activity for 2-CP hydration was found to be closely associated with the total basicity of the catalysts, and in turn a higher hydration rate was more conducive to the DMC synthesis through enhancing in-situ water removal efficiency. As expected, the present work provides in-depth insights into the structure-performance relationship of Fe-modified ceria-based catalysts for direct DMC synthesis from CO2 and methanol, and offers meaningful guidance for the advancement of highly efficient catalysts.
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