PHYSICAL CHEMISTRY CHEMICAL PHYSICS
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2020
·Vol. 22
·期 14
·7218-7223
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IF 3.43
Mengyao Lv,Haichuan Guo,Hangjia Shen,Jun Wang,Jiacheng Wang,Yuichi Shimakawa,Minghui Yang
A key challenge in carrying out an efficient oxygen reduction reaction (ORR) is the design of a highly efficient electrocatalyst that must have fast kinetics, low cost and high stability for use in an energy-conversion device (e.g. metal–air batteries). Herein, we developed a platinum-free ORR electrocatalyst with a high surface area and pore volume via a molten salt method along with subsequent KOH activation. The activation treatment not only increases the surface area to 940.8 m2 g−1 by generating lots of pores, but also promotes the formation of uniform Fe3C nanoclusters within the atomic dispersed Fe–Nx carbon matrix in the final material (A-FeNC). A-FeNC displays excellent activity and long-term stability for the ORR in alkaline media, and shows a greater half-wave potential (0.85 V) and faster kinetics toward four-electron ORR as compared to those of 20 wt% Pt/C (0.83 V). As a cathode catalyst for the Zn–air battery, A-FeNC presents a peak power density of 102.2 mW cm−2, higher than that of the Pt/C constructed Zn–air battery (57.2 mW cm−2). The superior ORR catalytic performance of A-FeNC is ascribed to the increased exposure of active sites, active single-atom Fe–N–C centers, and enhancement by Fe3C nanoclusters.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
·
IF 4.939
Mingxuan Fu,Qi Zhang,Yuena Sun,Guyang Ning,Xinyu Fan,Haiyang Wang,Haijun Lu,Yufan Zhang,Huan Wang
Electrochemical water-splitting is widely regarded as one of the essential strategies to produce hydrogen energy, while Metal-organic frameworks (MOFs) materials are used to prepare electrochemical catalysts because of its controllable morphology and low cost. Herein, a series of trimetallic porous Pt-inlaid Ni–Fe nanocubes (NCs) are developed with bifunctions of hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). In the process of prepare the electrochemical catalysts, Pt nanoparticles are uniformly embedded in the Fe–Ni PBA cube structure, and ascorbic acid is employed as a reducing agent to reduce Pt 2+ to Pt nanoparticles. In this work, the cubic structure of Fe–Ni PBA is maintained and the noble metal Pt nanoparticles are embedded. Remarkably, the formation of PBA cubes, Pt inlay and reduction are completed in one step, and Pt nanoparticles are embedded by a simple method for the first time. By employing acid etching method, a porous structure is formed on the PBA cube, which increases the exposed area of the catalyst and provides more active sites for HER and OER. Due to the porous structure, highly electrochemical active surface area and the embedded of highly dispersed Pt nanoparticles, the porous 0.6 Ni–Fe–Pt nanocubes (NCs) exhibits excellently electrocatalytic performance and durable stability to HER and OER. In this work, for HER and OER, the Tafel slopes are 81 and 65 mV dec −1 , the overpotential η at the current density of 10 mA cm −2 are 463 and 333 mV, and the onset potential are 0.444 and 1.548 V, respectively. And after a 12-h i-t test and 1000 cycles of cyclic voltammetry (CV), it maintained high stability and durability. This work opens up a new preparation method for noble metal embedded MOF materials and provided a new idea for the preparation of carbon nanocomposites based on MOF.
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JOURNAL OF ORGANIC CHEMISTRY
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2020
·
IF 4.335
Zhiwei Chen,Xiang Bai,Jie Sun,Yicheng Xu
A facile Fe(III)-catalyzed oxidative decarboxylative radical coupling reaction of α,α-difluoroarylacetic acids with coumarins has been developed. This transformation, which provides a series of C-3 difluoroarylmethylated coumarins containing various functional groups in moderate-to-good yields, features easily accessible starting materials and operational simplicity.
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APPLIED CLAY SCIENCE
·
2021
·
IF 5.467
Zhou Cao,Yuefa Jia,Qizhao Wang,Hongfei Cheng
Traditional homogeneous Fenton reactions can only be carried out under acidic conditions; however, visible light can greatly enhance the activity and stability of iron-doped semiconductor catalysts in the Fenton system. Therefore, in this study, a commercially applicable Fe/graphitic carbon nitride (g-C 3 N 4 )/kaolinite composite photocatalyst was prepared for the first time using an in-situ calcination process. The results showed that Fe ions and g-C 3 N 4 were successfully loaded onto kaolinite with a two-dimensional uniform sheet structure. The as-synthesized Fe/g-C 3 N 4 /kaolinite composite containing 0.9 mmol of Fe (Fe/CN/K-0.9) showed a degradation efficiency of 89% for tetracycline hydrochloride (TCH) within 80 min in the photo-Fenton system. Compared with photocatalytic degradation (29.6%) and Fenton degradation (76.6%), a photo-Fenton degradation efficiency of 85% was maintained after three cycles. Free radical scavenging experiments also showed that hydroxyl radicals were the main active substances. The enhanced photocatalytic activity of the composite was attributed to the large specific surface area of kaolinite, which could effectively adsorb TCH. Furthermore, Fe III acted as a photo-generated electron acceptor , which not only avoided photo-generated electron-hole recombination but also effectively reduced the consumption of H 2 O 2 to realize a stable Fe II /Fe III cycle reaction, thus improving photo-Fenton catalytic activity .
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COLLOIDS AND SURFACES B-BIOINTERFACES
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2021
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IF 5.268
Pu Zhang,Wanqiang Xia,Ping Deng,Yuanhong Min,Juan Tan,Yi Wang,Wensheng Fu
Peroxidase-like activity of MoS 2 quantum dots (QDs) can be reversibly regulated by means of Fe 3+ /alendronate sodium (ALDS)-induced aggregation/disaggregation of the QDs in solution. Specifically, Fe 3+ can selectively aggregate the MoS 2 QDs and thus greatly enhance their peroxidase-like activity, while such enhancement can be inhibited in the presence of ALDS owing to the competitive coordination of ALDS with Fe 3+ . By regulating the enzyme-like activity of MoS 2 QDs, different colorimetric signal of a typical substrate of horseradish peroxidase , 3,3΄,5,5΄-tetramethylbenzidine, can be measured in the presence of H 2 O 2 . Based on this mechanism, we develop a colorimetric approach for the determination of ALDS and further applied in quality control of pharmaceutical products, utilizing either smartphone or UV–vis spectrometer as a readout. This detection method is rapid and selective, where derivatization of ALDS before detection is not needed. Such a smartphone-based colorimetric detection platform is promising to be applied in point-of-care testing at home, small clinics, or underdeveloped regions.
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Biomass Conversion and Biorefinery
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2021
·Vol. 13
·期 9
·8115-8121
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IF 4.987
Ren Dezhang,Jiang Xuelei,Zhang Nahui,Duo Jia,Norinaga Koyo,Huo Zhibao
Production of pyridine derivatives from bio-based feedstocks instead of fossil fuels is a promising strategy. The development of effective heterogeneous catalysts and mild reaction systems for pyridinization of renewable biomass derivatives remains a huge challenge. In this article, a direct and environment-friendly method was reported to produce 3-hydroxypyridine from bio-based furfural in water over a Raney Fe catalyst. Raney Fe exhibited an efficient catalytic performance for activation of the aldehyde group of furfural and afforded an 18.2% yield of 3-hydroxypyridine at 120 °C with ammonia as N source. The polymerization of furfural on the catalyst in hot water was the main cause of deactivation, which was verified by the scanning electron microscope (SEM), X-ray diffraction (XRD), and N 2 adsorption and desorption analysis. A possible mechanism for this reaction was also proposed. This study provides a new way for academia and industry to realize the synthesis of nitrogen-containing chemicals from biomass and its derivatives.
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Bioactive Materials
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2021
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IF 14.593
Yunhang Liu,Bolong Xu,Mingzhu Lu,Shanshan Li,Juan Guo,Fangzhou Chen,Xiaolu Xiong,Zhe Yin,Huiyu Liu,Dongsheng Zhou
Pathogenic bacteria pose a devastating threat to public health. However, because of the growing bacterial antibiotic resistance, there is an urgent need to develop alternative antibacterial strategies to the established antibiotics. Herein, iron-doped carbon dots (Fe-CDs, ∼3 nm) nanozymes with excellent photothermal conversion and photoenhanced enzyme-like properties are developed through a facile one-pot pyrolysis approach for synergistic efficient antibacterial therapy and wound healing. In particular, Fe doping endows CDs with photoenhanced peroxidase (POD)-like activity, which lead to the generation of heat and reactive oxygen species (ROS) for Gram-positive and Gram-negative bacteria killing. This study demonstrates Fe-CDs have significant wound healing efficiency of Fe-CDs by preventing infection, promoting fibroblast proliferation, angiogenesis, and collagen deposition. Furthermore, the ultrasmall size of Fe-CDs possesses good biocompatibility favoring clinical translation. We believe that the nanozyme-mediated therapeutic platform presented here is expected to show promising applications in antibacterial.
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Energy Storage Materials
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2019
·
IF 0
Tao Dai,Lie Yang,Xiaohui Ning,Danli Zhang,R. Lakshmi Narayan,Ju Li,Zhiwei Shan
Due to their compactness, storage/supply flexibility, modularity and factory manufacturability, batteries are excellent candidates for large scale energy storage applications . However, the widespread application of most batteries hitherto developed is hindered by their high cost. Here, an intermediate temperature molten salt battery is developed that emphatically resolves this issue by using all earth-abundant and cheap elements. Operated at 170 °C, the cell comprises of an Fe metal anode, NaCl saturated NaAlCl 4 electrolyte and an AlCl 4 − intercalated graphite cathode in the fully charged state. It has a capacity retention of 85% after nearly 10,000 cycles. After characterizing the anode, it was determined that the high reversibility of the Fe to FeCl 2 solid state transformation are responsible for the absence of dendritic growth on such a metal anode. Different electrode capacity matching strategies are discussed in the context of ensuring safe operation during overcharging. Finally, the overall material cost of the Fe/Graphite cell is estimated to be 33.9 $ kWh −1 , which can potentially meet the demands of the commercial energy storage market.
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Journal of Analysis and Testing
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2019
·Vol. 3
·期 3
·238-245
·
IF 0
Sun Shihao,Fan Yaofang,Du Jiaoyang,Song Zhilian,Zhao Huimin
Over the past few decades, the enzyme-mimicking activity of metal–organic frameworks (MOFs) accompanied with structural characteristics has aroused much attention. However, pure MOFs have low affinity with DNA. Here, iron-based MOFs with acidized carbon nanotubes (CNTs) via a simple hydrothermal process have been synthesized, named as MIL-88(NH 2 )-Fe@CNTs. CNTs can enhance the affinity between MOF and DNA, achieving flexible regulation of their catalytic activity benefiting from the strong π − π stacking between CNTs and DNA. Meanwhile, in comparison with conventional iron-based MOFs, the addition of CNTs, which contributes to the acceleration of electron transfer, endowing as-prepared nanocomposites remarkably enhanced peroxidase-like activity to achieve an ultrasensitive detection of H 2 O 2 with the LOD of 17.64 μg/L. Notably, the as-prepared nanocomposites with adsorbed DNA displayed excellent affinity towards both TMB (3, 3′, 5, 5′-tetramethylbenzidine) substrates and H 2 O 2 as well as high catalytic velocity. On the basis of their switchable peroxidase-like activity regulated by different length or sequence of ssDNA, it is believed that our-prepared MOF-based nanomaterials would be promising for fabricating versatile and sensitive label-free colorimetric assays for diverse targets.
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ACS Applied Materials & Interfaces
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2019
·
IF 8.456
Yuda Zhu,Nini Xin,Zi Qiao,Suping Chen,lingwan Zeng,Yusheng Zhang,Dan Wei,Jing Sun,Hongsong Fan
Traditional tumor treatments suffer from severe side effects on account of their invasive process and inefficient outcomes. Featuring a unique physical microenvironment, the tumor microenvironment (TME) provides a new research direction for designing more efficient and safer treatment paradigms. In this study, we fabricated a polydopamine (PDA)-based TME-responsive nanosystem, which successfully integrates glucose degradation, the Fenton reaction, and photothermal therapy for efficient cancer therapy. Through a convenient hydrothermal method, Fe2+-doped Fe(II)–PDA nanoparticles were successfully fabricated, which show an excellent photothermal effect and interesting reactivity for the Fenton reaction. Instead of introducing toxic anticancer agents, natural glucose oxidase (GOD) was grafted on Fe(II)–PDA, forming a cascade catalytic nanomedicine for a specific response to the glucose in TME. GOD grafted on Fe(II)–PDA–GOD is ought to catalyze abundant glucose in TME into gluconic acid and H2O2. The concomitant generation of H2O2 can enhance the efficiency of the sequential Fenton reaction, producing abundant hydroxyl radicals (•OH) for cancer therapy. Besides, the overconsumption of intratumoral glucose also could inhibit tumor growth by reducing the energy supply. Taken together, the in vitro and in vivo antitumor studies of such TME-based Fe(II)–PDA–GOD nanosystems displayed a favorable synergistic potency of glucose degradation, the Fenton reaction, and photothermal therapy against tumor growth. Our design expands the biological application of multifunctional PDA while providing novel strategies toward effective antitumor treatment with minimal side effects.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2019
·
IF 6.361
Fuqin Zheng,Ziwei Zhang,Dong Xiang,Ping Li,Cheng Du,Zhihua Zhuang,Xiaokun Li,Wei Chen
Electrochemical water-splitting is an ideal strategy to produce the promising substitutable energy source, hydrogen (H 2 ). However, the sluggish kinetics of electrochemical oxygen evolution reaction (OER) and the prohibitive cost, low reserves and easy oxidation of noble metal-based electrocatalysts force researchers to explore efficient and low-cost electrocatalysts . Bimetal nanostructred materials are proved to have enhanced OER catalytic performances. In this study, a series of bimetallic metal-organic frameworks (Fe/Ni-MOFs) are prepared by a solvothermal method . The prepared MOFs present abundant unsaturated metal active sites for OER. The optimized Fe/Ni bimetal-MOF has low overpotentials of 236 mV at 10 mA cm −2 and 284 mV at 100 mA cm −2 for OER. In addition, in comparison with most of the previously reported OER electrocatalysts, the present MOF shows a lower Tafel slope of 49 mV dec −1 . Besides, the MOF catalyst exhibits high electrochemical stability and the OER activity shows a negligible change after stability test for 15 h and 10,000 voltammetric cycles. Meanwhile, the Fe-doped Ni-MOFs show faster catalytic kinetics and higher conductivity than the monometallic Ni-MOF. This work paves a way to exploit bi- or multi-metallic MOFs with high conductivities and electrocatalytic performances for electrochemical energy conversion .
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CHEMICAL ENGINEERING SCIENCE
·
2019
·
IF 3.372
Mingyue Liu,Renliang Huang,Chuanxi Li,Mingda Che,Rongxin Su,Shuzhou Li,Jing Yu,Wei Qi,Zhimin He
Nanoscale zero-valent iron has been widely applied in environmental remediation and toxic waste treatment, especially for the degradation of persistent organic pollutants (POPs). However, the dechlorination activity of Fe nanoparticles (Fe NPs) can be suppressed by the precipitation of iron oxides generated from the corrosion of Fe-Pd NPs under alkaline conditions, leading to a decreased dechlorination efficiency. Faced with this challenge, we report a highly effective dechlorination system that functions over a broad pH range and especially well under alkaline conditions in this work. Procyanidin (PROC), a natural polyphenol, was utilized as a stabilizer to manipulate the size distribution of Fe-Pd NPs and, more importantly, as a scavenger of Fe ions to prevent iron oxide precipitation. Experiments and theoretical calculations reveal that the generated Fe ions was mainly present in the form of bis- and tris-PROC-Fe complexes in the reaction solution. Compared with pristine Fe-Pd NPs, the PROC-modified Fe-Pd NPs had a dechlorination efficiency that was increased 20-fold (pH 9.0). Notably, a normalized rate constant was enhanced by more than 2 orders of magnitude compared to the previously reported dechlorination systems. The PROC-modified Fe-Pd NPs showed excellent dechlorination efficiency over a wide pH range (2.3–13.0).
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