ACS Applied Materials & Interfaces
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2021
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IF 9.229
Changyang Liu,Shuting Li,Jianquan Gao,Liuzhen Bian,Yunting Hou,Lijun Wang,Jun Peng,Jinxiao Bao,Xiwen Song,Shengli An
The development of cathode materials with high catalytic activity and low cost is a challenge for CO2 electrolysis based on solid oxide electrolysis cells. Herein, we report a low-cost and highly active metallic Fe nanoparticle-decorated Ruddlesden-Popper (La, Sr)FeO4+δ cathode catalyst (Fe-RPLSF), which shows a high oxygen vacancy concentration and robust CO2 reduction rate. At 850 °C, the current density of the electrolysis cell with the Fe-RPLSF cathode reaches −1920 mA cm–2 at a voltage of 1.5 V, and the Faraday efficiency is as high as 100%. The polarization resistance at low frequency (0.1–10 Hz), which is the rate-limit step for CO2 electrolysis, significantly decreases with the exsolved Fe nanoparticles because of improved CO2 dissociative adsorption. Moreover, our electrolysis cell demonstrates acceptable short-term stability for direct CO2 electrolysis.
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ELECTROCHIMICA ACTA
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2020
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IF 6.215
Wenhui Fang,Jing Wang,Ye Hu,Xiaoqing Cui,Ruifeng Zhu,Yuhua Zhang,Chaochao Yue,Jiaqi Dang,Wei Cui,Hong Zhao,Zengxi Li
It's a major challenge to explore highly active and stable electrocatalysts for efficient hydrogen evolution reactions (HER) and oxygen evolution reactions (OER). In this work, we report a new hybrid electrocatalyst: iron-cobalt decorated nitrogen doped carbon/reduced graphene oxide-700 °C (Fe-Co-CN/rGO-700). The catalyst shows an excellent electrocatalytic performance toward HER and OER in alkaline solution, which has lower overpotentials of 0.215 V and 0.308 V at the current density 10 mA cm −2 , respectively, and this catalyst has an outstanding durability (after 45 h). The excellent activity mainly benefit from the highly dispersed iron/cobalt species, sheet structure with high porosity, the improvement of electronic structures with nitrogen-doped carbon and high conductivity of rGO. Combined with the density function theory (DFT) calculations, the improvement of the HER and OER performance were also attributed to the balance of adsorption/desorption of the hydrogen and oxygen-containing intermediates, and the increased electronic states density near the Fermi level. The proposed work provides a novel and simple strategy to synthesize a porous carbon electrocatalyst material using metal-organic frameworks (MOFs) as precursor with high activity and strong stability for HER and OER.
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Journal of Water Process Engineering
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2021
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IF 5.485
Jialin Chen,Ruina Zhang,Dong Chen,Jianyong Liu,Shanping Chen
The generation process for the highly reductive carbon dioxide radical ( CO 2 − ) in the Fe(III)-oxalate system is enhanced under UV irradiation and used in nitrate (NO 3 − ) reduction with improved product selectivity to nitrogen (N 2 ). The combination of Fe(III) and residual oxalate forms Fe(III)-oxalate complexes again for an Fe(II)/Fe(III) species cycle and achieves generation of CO 2 − radical continually. The electron paramagnetic resonance (EPR) spectrum demonstrates the existence of CO 2 − radicals in this process. Some of the important control factors, such as initial concentrations of ferric ions (Fe(III)) (0.5, 1, 2, and 3 mM), NO 3 − (14, 21, and 42 mg N/L), oxalate (3, 7, and 10 mM), and pH values (2, 3, 4, 5, and 6), are systematically assessed for NO 3 − reduction efficiency and N-species selectivity. Among all the control factors mentioned, pH is a key parameter with an important role in the NO 3 − reduction process. Excellent NO 3 − reduction efficiency (∼90 %) was achieved at pH 3 in the presence of 1 mM Fe(III) and 10 mM oxalate under UV irradiation for 120 min. High Fe(III) and oxalate concentrations promote NO 3 − removal. In addition, there was an increase in the NO 3 − removal amount with a greater initial NO 3 − concentration. About 60 % of NO 3 − can be selectively reduced to N 2 with low selectivity to NO 2 − (∼3.4 % of total N) and NH 4 + (∼15.7 % of total N). In general, the UV/Fe(III)-oxalate system provided an alternative way to improve NO 3 − removal performance and selectivity to form N 2 in water and wastewater remediation processes.
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ACS Applied Materials & Interfaces
·
2020
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IF 8.758
Bing Wang,Yeneng Dai,Yingjie Kong,Wenyu Du,Haiyang Ni,Honghai Zhao,Zhiquan Sun,Qingming Shen,Meixing Li,Quli Fan
The development of effective and safe tumor nanotheranostics remains a research imperative. Herein, tumor microenvironment (TME)-responsive Fe(III)–porphyrin (TCPP) coordination nanoparticles (FT@HA NPs) were prepared using a simple one-pot method followed by modification with hyaluronic acid (HA). FT@HA NPs specifically accumulated in CD44 receptor-overexpressed tumor tissues through the targeting property of HA and upon endocytosis by tumor cells. After cell internalization, intracellular acidic microenvironments and high levels of glutathione (GSH) triggered the rapid decomposition of FT@HA NPs to release free TCPP molecules and Fe(III) ions. The released Fe(III) ions could trigger GSH depletion and Fenton reaction, activating chemodynamic therapy (CDT). Meanwhile, the fluorescence and photodynamic effects of the TCPP could be also activated, achieving controlled reactive oxygen species (ROS) generation and avoiding side effects on normal tissues. Moreover, the rapid consumption of GSH further enhanced the efficacy of CDT and photodynamic therapy (PDT). The in vivo experiments further demonstrated that the antitumor effect of these nanotheranostics was significantly enhanced and that their toxicity and side effects against normal tissues were effectively suppressed. The FT@HA NPs can be applied for activated tumor combination therapy under the guidance of dual-mode imaging including fluorescence imaging and magnetic resonance imaging, providing an effective strategy for the design and preparation of TME-responsive multifunctional nanotheranostics for precise tumor imaging and combination therapy.
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Arabian Journal of Chemistry
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2020
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IF 4.762
Zijun Dong,Feng Wang,Xiulan Song,Miao Zhang,Chengchun Jiang,Feiyun Sun,Mu Li
Iodoform (CHI 3 ) is one of the disinfection by-products (DBPs) that is formed in the pre-oxidation and disinfection processes of drinking water treatment. In this study, Fe(II)-activated persulfate oxidation (Fe 2+ /PS) was employed to degrade iodoform, the effects of initial reactants concentration, reaction parameters, kinetics model were investigated, and the underlying mechanisms of CHI 3 degradation in Fe 2+ /PS oxidation process was unveiled. The results showed that the mole ratio Fe 2+ /PS of 1:5, initial PS concentration of 15 μmmol/L, and pH of 3.0 were identified as the optimum operating parameters. In addition, a relatively higher temperature could enhance CHI 3 removal and deiodination. The kinetic model has two different reaction steps: a fast one during the first ten minutes of reaction; then followed by a much slower one. Suppression of the reaction by TBA and MeOH showed that the combined effects of SO 4 − · and ·OH contributed to the degradation of CHI 3 , but ·OH played a dominant role. The degradation pathways and the products of total liberated iodine species demonstrate that the applicability of the Fe 2+ /PS oxidation process for CHI 3 degradation. These results indicated that the Fe 2+ /PS oxidation process is an effective advanced oxidation process for CHI 3 removal in water treatment.
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Journal of Materials Chemistry A
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2020
·Vol. 8
·期 8
·4369-4375
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IF 11.301
Lulu Chen,Yelong Zhang,Lile Dong,Wenxiu Yang,Xiangjian Liu,Ling Long,Changyu Liu,Shaojun Dong,Jianbo Jia
Rational design of isolated metal atom doped carbon catalysts is essential for revealing the essence of high activity for the oxygen reduction reaction (ORR), which can promote the development of robust catalysts for clean energy conversion devices. Herein, we report a simple one-step strategy to prepare Fe and Co atomically supported on N-doped nanocarbon (FeCo-IA/NC) from metal–organic frameworks with excellent ORR activity. The isolated Fe–N4 and Co–N4 sites are characterized by atomic-resolution aberration-corrected scanning transmission electron microscopy and X-ray absorption fine structure spectroscopy. The electrochemical results and density functional theory calculations indicate that the synergetic effect between Fe–N4 and Co–N4 accounts for the enhanced ORR activity. Benefiting from the large BET surface area, microporous feature, and high content (85%) of pyridinic and graphitic N, the well-designed catalyst exhibits better ORR activity (half-wave potential of 0.88 V) and Zn–air battery performances (higher open circuit potential and power density) than commercial Pt/C. This work may lay a foundation for further exploring efficient non-precious metal-based catalysts for the ORR and developing clean energy conversion devices.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Zhuozhi Ouyang,Chen Yang,Junheng He,Qian Yao,Bijie Zhang,Hanming Wang,Yu Jiang,Jini Zhou,Yurong Deng,Yanjun Liu,Jingjing Yang,Guining Lu,Zhi Dang
Sulfamethazine (SMT), taken as model compound, have been exposed to a photocatalytic system driven by ultraviolet light (UV) irradiation with Fe(III) and three carboxylic acids (citric, tartaric and malic acid). The kinetic experiments, quenching experiments, electron paramagnetic resonance (EPR), species model theoretical calculation, density functional theory (DFT) and intermediates analyses, were conducted to analyze the formation of reactive oxygen species (ROS) and underlying mechanism of Fe(III)-carboxylate complexes on photocatalytic degradation of SMT. The results indicated the complexes easily induced the degradation under UV irradiation. Enough hydroxyl radicals ( · OH) were produced and the singlet oxygen ( 1 O 2 ) originated from the self-sensitized oxidation. An interaction among ROS, Fe(III)-carboxylate complexes and SMT was firstly proposed. The active sites and groups were characterized through Frontier electron densities (FEDs), Fourier Transform-Infrared (FTIR) and Two-dimensional correlation FTIR spectroscopy (2D-FTIR-CoS) analyses. The transformation pathway mainly included four reactions: hydroxylation, SO 2 extrusion, Smiles-type rearrangement and S-N bond cleavage. The system also had an application potential for removing SMT from practical water.
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ANALYTICA CHIMICA ACTA
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2020
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IF 5.977
Xiaobin Zhou,Mengke Wang,Junyang Chen,Xiaolei Xie,Xingguang Su
Single atom nanozymes are the artificial enzymes with enzyme-like activity, which have attracted a great deal attention in recent years due to their unique merits such as remarkable stability, excellent atom utilization and low cost. Herein, a convenient and sensitive colorimetric strategy was developed for the sensing of galactose based on Fe–N–C single-atom nanozyme (Fe-SAzyme). The Fe-SAzyme was prepared through “isolation-pyrolysis” method that exhibited intrinsic peroxidase mimicking activity, which can quickly catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to produce blue-colored oxTMB in the presence of hydrogen peroxide (H 2 O 2 ). Galactose can be oxidized by galactose oxidase (Gal Ox) to generate H 2 O 2 , and Fe-SAzyme can be utilized for quantitative colorimetric detection of galactose. A good linearity between absorbance and the galactose concentration in the range of 50–500 μM was obtained with a detection limit of (LOD) 10 μM. The Fe-SAzyme based colorimetric strategy offered a rapid, convenient and economic way for galactose quantification detection, which could be used as an alternative method for galactosemia diagnosis.
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ACS Omega
·
2020
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IF 2.87
Tianzhao Hu,Jiafu Chen,Xiaoqing Lu,Jing Chen,Zhimin Chen,Jianwei Fu,Yong Chen
Graphene sheets have a vast number of potential applications due to their excellent properties. However, poor quality and harsh preparation conditions restrict their application. Here, few-layer graphene (FLG) sheet powder with high quality has been synthesized from waste expanded polystyrene (EPS) at low temperature by dense Fe cluster catalysis. The micron-sized FLG sheets comprising about three layers show high crystallinity and good electrical conductivity that are comparable to those of the shear-exfoliated graphene nanoplatelets. More than 70% carbon yield of FLG sheets from cheap EPS and their safe, controllable synthesis conditions make it easy to expand production. The catalytic formation mechanism of FLG sheets is studied.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2020
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IF 3.807
Xiaoying Zhai,Weiguo Lin,Jinkai Liu,Xu Chen,Junfeng Yong,Wensheng Yang
The development of earth-abundant electrocatalysts to replace noble metal for oxygen reduction reaction (ORR) has attracts tremendous interest. In this work, Fe, N-codoped porous carbon-embedded Fe 3 C nanoparticles (Fe 3 C/Fe, N-PCR) is fabricated from petroleum vacuum residue via a simple template-assisted and subsequent doping-assisted calcination method. The unique hybrid material shows great features: abundant active sites including pyridinic N, Fe N, and Fe 3 C nanoparticles, a relatively large surface area (509.3 m 2 g − 1 ) and 3D interconnected hierarchical porous structure. The Fe 3 C/Fe, N-PCR as an electrocatalyst exhibits remarkable ORR catalytic activity in alkaline medium, with a high onset potential of 1.02 V and half-wave potential of 0.86 V, which surpass commercial Pt/C (20 wt%) by ca. 30 and 20 mV, respectively. Moreover, Fe 3 C/Fe, N-PCR has outstanding long-term stability and tolerance to methanol poisoning, outperforming Pt/C. Combining with the exciting performance, abundant and cheap raw material, and facile synthetic method, Fe 3 C/Fe, N-PCR catalyst has promising future in ORR. This study also provides a new approach for high value utilization of petroleum vacuum residue.
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Scientific Reports
·
2020
·Vol. 10
·期 1
·1-9
·
IF 3.998
Zhang Lei,Weng Yi-jin,Liu Xiao,Gu Wen,Zhang Xia,Han Lei
Surface Enhanced Raman Scattering (SERS) has been widely applied in many research fields such as biological detection and chemical analysis. However, for the common Au nanoparticles, it’s too hard to guarante the three aspects: the great enhanced effect, the controllable aggregation and the uniformity of nanoparticles, the environmental friendliness and biocompatibility of nanoparticles. In this paper, phytate acid (IP6)-coated Au nanoparticles (IP6@Au NPs) are more stable and have a higher enhancement factor than Au nanoparticles. In order to achieve the uniformity of the spherical IP6-coated@Au nanoparticles (IP6@Au NPs), IP6 was used as a soft template. In the presence of IP6, IP6@Ag nanoparticles were first synthesized by reducing AgNO 3 with trisodium citrate, then IP6@Au NPs were obtained by reducing HAuCl 4 with Ag nanoparticles. The IP6@Au NPs exhibit excellent Raman signal enhancement by using p-aminothiophenol (4-ATP) as the probe molecules. The effects of Fe 3+ on the performance of IP6@Au NPs SERS substrates were also studied. The results show that SERS has the best enhancement effect when adding proper amount of Fe 3+ (0.56 PPM), and the limit of detection was 10 −7 M 4-ATP.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2020
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IF 4.65
Yanyan Wu,Ying Li,Mengke Yuan,Zhe Lü,Lingling Xu,Bo Wei
Developing efficient and nonprecious electrocatalysts for oxygen evolution reaction (OER) is crucial for the hydrogen generation via water splitting. Here we report the direct growth of heterostructural Ni 2 P–Fe 2 P hybrid electrocatalysts on NiFe foams. The redox engineered NiFe foam (rNF) significantly enhances the OER performance. Among prepared catalysts, Ni 2 P–Fe 2 P/rNF performs the highest OER activity, driving the current densities of 10 and 100 mA cm −2 at low overpotentials of 218 and 270 mV in 1 M KOH, respectively. Meanwhile, it can maintain 100 mA cm −2 for 24 h without obvious degradation. The morphology and composition of NFP/rNF after OER test were carefully studied. This work suggests that self-supported bimetal phosphides of NFP/rNF is an efficient and durable electrode material for water oxidation .
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