ACS Applied Materials & Interfaces
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2022
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IF 10.383
Ziyang Huang,Siyi Zou,Guozhen Liu
It is a long-lasting research topic to avoid the formation of oxidation layers on gallium-based liquid metals. This study has developed a simple general method for modification of the eutectic gallium–indium (EGaIn) surface with p-aniline derivatives to introduce a monolayer of organic molecules with versatile functional groups. The binding affinity of carboxylic acid groups, amine groups, or thiol groups with EGaIn is in the order SH > NH2 > COOH. For the first time, it is evidenced that both NH2 and SH groups can coexist on the EGaIn nanoparticle surface with the binding affinities of 30 and 70%, respectively. The formation of these organic molecules on the EGaIn surface antioxidizes and thus stabilizes the EGaIn nanoparticles, while increasing the conductivity of EGaIn significantly. The resulting EGaIn nanoparticles have very good distribution in both ethanol and aqueous solutions and rich surface chemistry, making them suitable for the following attachment of biomolecules such as aptamers, antibodies, or enzymes for biomedical applications. As an example, the EGaIn surface is successfully modified with p-aminobenzoic acid followed by the attachment of an insulin aptamer, which can be used for the electrochemical detection of insulin with the lowest detectable concentration limit of 1 pM. This study reveals the modification of EGaIn nanoparticles with p-aniline derivatives with versatile functional groups to antioxidize EGaIn in a biological environment, opening a door for gallium-based liquid metals toward biomedical applications.
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ENVIRONMENTAL TECHNOLOGY
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2022
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IF 3.475
Yafang Zhang,Shuning Yang,Linsheng Wei,Xiaoyang Zhao,Xiangdong Lu
Photocatalysis is a promising technology for wastewater treatment. It is of great significance to find catalysts with high photoactivity. In this paper, a catalyst with high photocatalytic degradation efficiency to organic wastewater, carbon nitride modified by graphene quantum dots (SCN-GQDX), is prepared by supramolecular self-assembly thermal polycondensation method and doping graphene quantum dots (GQDs). The results show that SCN-GQD0.5 has the best catalytic performance, and its photocatalytic degradation efficiency to organic pollutants can reach 86% and still remains above 83% after five cycles, which shows the modified carbon nitride has high catalytic efficiency and stability. In a word, SCN-GQDX is a highly efficient, non-toxic and stable photocatalyst for organic pollutants in wastewater.
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MICROCHEMICAL JOURNAL
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2022
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IF 5.304
Xue Wang,Mengjia Li,Shuang Yang,Xuting Bai,Jiajia Shan
p -Nitrophenol ( p -NP) is an important phenolic environmental pollutant. The development of novel rapid determination methods for p -NP is of significance for environmental monitoring. In this work, a sensitive electrochemical sensor based on Ti 3 C 2 T X MXene/graphene composite was developed to detect p -NP in aqueous samples. Firstly, delaminated titanium carbide (D-Ti 3 C 2 T X ) was successfully prepared via an optimized minimally intensive layer delamination (MILD) method, which was further followed by the self-assembly method to form D-Ti 3 C 2 T X /graphene (D-Ti 3 C 2 T X /GR) composite. The prepared materials were characterized by scanning electron microscopic (SEM), X-ray diffraction (XRD), atomic force microscopy (AFM) and Raman spectroscopy. Then the glassy carbon electrode (GCE) was modified by D-Ti 3 C 2 T X /GR composite to prepare the D-Ti 3 C 2 T X /GR/GCE sensor. The electrochemical behavior of D-Ti 3 C 2 T X /GR/GCE was investigated by cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), and chronocoulometry. Furthermore, the proposed sensor showed a strong electrochemical response based on the p -NP reduction reaction, benefiting from abundant active sites, fast electron transfer, and excellent electro-catalytic performance of the D-Ti 3 C 2 T X /GR composite. Under the optimal conditions, the D-Ti 3 C 2 T X /GR based electrochemical sensor displayed a linear response in the p -NP concentration range from 1 to 175 μmol·L −1 with a detection limit of 0.16 μmol·L −1 . The anti-interference performance, reproducibility, stability, and recovery in real sample analysis were also further evaluated. This study provided a novel and sensitive method for the rapid determination of p -NP in environmental samples.
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ACS Applied Energy Materials
·
2022
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IF 6.959
Guangzhou Hu,Wenying Fu,Yuxiao Lin,Yuanchao Yue,Maosen Wang,Pengbo Liu,Yinwei Li,Jianwei Li,Lu Wei,Xinsheng Zhao,Yongsheng Wei
Electrochemical water splitting to produce clean hydrogen (H2) and oxygen (O2) has emerged as an advanced technology to build a sustainable society. Low-cost electrocatalysts with excellent performance are required to improve the energy efficiency in overall water splitting. Here, a Co-W-B-P/CF catalyst with a nanoflower-like structure consisting of microspheres and nanoflakes was successfully synthesized using a one-step double-pulse electrodeposition approach. When used as a bifunctional electrocatalyst for overall water splitting, Co-W-B-P/CF presented the potentials of 1.57 and 1.86 V at current densities of 10 and 100 mA cm–2 in 1.0 M KOH solution, respectively. This was even comparable to that of the high-cost commercial catalyst Pt/C(−)//IrO2(+). Detailed electrochemical tests also showed that the kinetics, electron transfer, and intrinsic electrocatalytic activity of Co-W-B-P/CF in the HER (hydrogen evolution reaction) and the OER (oxygen evolution reaction) were dramatically improved due to the synergetic effect of co-doped B and P elements. Considering the excellent electrocatalytic performance of Co-W-B-P/CF, along with the simple synthesis method and low cost, bifunctional electrocatalyst Co-W-B-P/CF for overall water splitting is promising.
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EUROPEAN POLYMER JOURNAL
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2022
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IF 5.546
Jun Chen,Cong Liao,Xiao-Xiao Guo,Shi-Chang Hou,Wei-Dong He
Lead ion is a common heavy metal pollutant and extremely harmful to human health. Therefore, the research about the adsorption and removal of lead ion from sewage and the development of lead ion sorbents keeps greatly significant. In this study, poly(acrylic acid- co -acrylonitrile) (PAAN) cryogels were prepared by cryo-polymerization. After the treatment with hydroxylamine, the amidoximated PAAO cryogels were applied to remove lead ion from lead-contaminated water. The porous structure and high water permeability of the cryogel could fully facilitate the exposure of active sites to efficiently adsorb lead ion. PAAO cryogels showed a high adsorption capacity of 450 mg/g for lead ion. After the first adsorption–desorption cycle, the adsorption capacity of PAAO cryogels regenerated with alkali solution increased to 650 mg/g and remained in the next six cycles. The pseudo-second-order kinetic model and the intraparticle diffusion model fit the adsorption kinetics of lead ion well, indicating its chemi-sorption feature of PAAO cryogel sorbent. The FTIR and XPS studies suggested that carboxyl group of acrylic acid unit as well as the amidoxime group of modified AN unit contributed the enhanced adsorption ability for lead ion.
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INORGANIC CHEMISTRY
·
2022
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IF 5.436
Jingsheng Zhou,Beibei An,Zhiyong Zhu,Li Wang,Jinglai Zhang
Doping heteroatoms in carbon materials is a promising method to prepare the robust electrocatalysts for the carbon dioxide reduction reaction (CO2RR), which is beneficial for sustainable energy storage and environmental remediation. However, the obscure recognition of active sites is the obstacle for further development of high-efficiency electrocatalysts, especially for the N,P-codoped carbon materials. Herein, a series of N,P-codoped carbon materials (CNP) is prepared with different N and P contents to explore the relationship between the N/P configuration and the CO2RR activity. As compared with the N-doped carbon materials, the additional P doping is helpful to improve the activity. The optimum N,P-codoped carbon materials (CNP-900) achieve 80.8% CO Faradaic efficiency (FECO) at a mild overpotential of 0.44 V. On the basis of the X-ray photoelectron spectroscopy results, the suitable ratio between pyridinic N and graphitic N and the least P–N content are beneficial for CO2RR. The density functional theory calculations further illustrate that two elementary steps to form *COOH and *CO in CO2RR are determined by the graphitic N and pyridinic N configurations, respectively. The existence of the P–N configuration breaks the equilibrium between graphitic N and pyridinic N to suppress the activity.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Xiang Mei,Han Gao,Yang Ding,Chao Xue,Lijie Xu,Yong Wang,Lei Zhang,Mengyuan Ma,Zimiao Zhang,Yanyan Xiao,Xu Yang,Chengqi Yin,Zhan Wang,Mengmeng Yang,Dongyu Xia,Cai Wang
Membrane biofilm (MBf) technology is a promising biological water treatment process that combines membrane aeration with biofilms. To expand its application in the treatment of toxic organic wastewater, methane/air gas mixture-MBfs ((CH 4 + Air)-MBfs) and air-MBfs were coupled to enhance the treatment of p -nitroaniline (PNA) wastewater. Based on exploration of the membrane permeability of methane and oxygen, a hybrid MBf reactor was constructed, and the degradation characteristics of PNA and the coupling effects of (CH 4 + Air)-MBfs and air-MBfs were studied. The permeation flux of methane was found to be 1.114 g/(m 2 d) when using a methane/air gas mixture at an aeration pressure of 10 kPa, and this result was better than that when methane was used as the aeration gas alone. Aeration with a methane/air gas mixture provided conditions for realizing aerobic methane oxidation ; the aerobic methane oxidation that occurred in the (CH 4 + Air)-MBfs promoted the reduction of PNA, and the intermediates of PNA degradation were further degraded by the air-MBfs. At an influent PNA membrane area load of 1.67 g/(m 2 d), the PNA removal load reached 187.30 g/(m 3 d). The coupling of MBfs took advantage of different matrix-based MBfs and promoted the degradation of PNA by utilizing the synergistic effects of various functional microorganisms .
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Yanyan Cui,Ping Zhang,Mengke Li,Chengcheng Lin,Yaling Wang
Photocatalysis technology is considered an effective way to solve the problem of water pollution and energy shortage, and is hinged on the development of the photocatalyst . In this study, p-type semiconductor AgFeO 2 and the n-type photocatalyst Ag 3 VO 4 formed a p-n junction via a simple hydrothermal method . Compared with pure Ag 3 VO 4 , the 4 % AgFeO 2 -modified Ag 3 VO 4 photocatalyst (AgVFe-4) exhibited the best photocatalytic activity: the photodegradation rate of RhB reached 95.1 % within 60 min and possessed good photostability under UV–visible light irradiation. The physical and chemical properties of AgVFe-4 indicated that the composite structure showed a larger special surface area, much lower intensity of photoluminescence , and higher photogenerated carriers separation efficiency. The p-type AgFeO 2 and n-type Ag 3 VO 4 could form the p-n junction structure. Based on the analysis of reactive agents, the h + , •O 2 − and •OH were the main active species during organic pollutions photodegradation, and the photocatalysis process followed the Z-scheme mechanism. Meanwhile, some silver element in the photocatalyst was reduced into Ag 0 , which could act as the recombination center of the photogenerated carriers, further improving the photocatalytic performance. This work may arouse an increasing interest in designing more Z-scheme silver-based p-n junction heterojunction photocatalysts.
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ChemSusChem
·
2022
·Vol. 15
·期 15
·e202200752
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IF 9.14
Helei Wei,Aidong Tan,Zhipeng Xiang,Jie Zhang,Jinhua Piao,Zhenxing Liang,Kai Wan,Zhiyong Fu
Graphical Ni doping enhances CO 2 reduction : The Ni doping dramatically modulated the electronic structure of the Bi nanosheet by increasing its p-orbital electronic density states and shifting towards the Fermi level. The resultant strong orbital hybridization between Bi and the π* orbitals of CO 2 facilitates the formation of *OCHO intermediates and favors its activation, leading to high activity and selectivity toward HCOOH during CO 2 electroreduction. Electrochemical reduction of CO 2 (CO 2 RR) to value-added chemicals is an effective way to harvest renewable energy and utilize carbon dioxide. However, the electrocatalysts for CO 2 RR suffer from insufficient activity and selectivity due to the limitation of CO 2 activation. In this work, a Ni-doped Bi nanosheet (Ni@Bi-NS) electrocatalyst is synthesized for the electrochemical reduction of CO 2 to HCOOH. Physicochemical characterization methods are extensively used to investigate the composition and structure of the materials. Electrochemical results reveal that for the production of HCOOH, the obtained Ni@Bi-NS exhibits an equivalent current density of 51.12 mA cm −2 at −1.10 V, which is much higher than the pure Bi-NS (18.00 mA cm −2 at −1.10 V). A high Faradaic efficiency over 92.0 % for HCOOH is achieved in a wide potential range from −0.80 to −1.10 V, and particularly, the highest efficiency of 98.4 % is achieved at −0.90 V. Both experimental and theoretical results reveal that the superior activity and selectivity are attributed to the doping effect of Ni on the Bi nanosheet. The density functional theory calculation reveals that upon doping, the charge is transferred from Ni to the adjacent Bi atoms, which shifts the p-orbital electronic density states towards the Fermi level. The resultant strong orbital hybridization between Bi and the π* orbitals of CO 2 facilitates the formation of *OCHO intermediates and favors its activation. This work provides an effective strategy to develop active and selective electrocatalysts for CO 2 RR by modulating the electronic density state.
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ChemistrySelect
·
2022
·Vol. 7
·期 31
·e202201268
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IF 2.307
Aixiao Fu,Mengqing Sun,Shifeng Jiang,Huanfei Xu,Guoqiang Xu
Graphical Pyrroles are important nitrogen-containing compound. Here, we constructed N, P-doped activated carbon supported Ir to perform the synthesis of pyrroles from alcohols and amino alcohols. The unique performance is attributed to the interaction between Ir and N, P-doped activated carbon. Pyrroles are a significant class of nitrogen-containing heterocyclic compounds and the derivatives. Here, an efficient procedure has been proposed for the loading of Ir on N, P-doped activated carbon to exploit pyrroles are synthesized from alcohols and amino alcohols. And the optimal conversion of 1-phenylethanol is up to 65 % with 2-phenylpyrrole selectivity of 80 %. The good performance is attributed to the interaction between metal Ir and N, P-doped activated carbon, which could also be confirmed from BET and XPS characterizations. What's more, the catalyst could be generally used for a range of reactions to produce pyrroles from alcohols and amino alcohols.
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JOURNAL OF APPLIED POLYMER SCIENCE
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2022
·Vol. 139
·期 37
·e52878
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IF 3.057
Jianhua Wu,Meng Li,Ying Cao,Jianmin He,Mingjin Xue,Aoqi Zhu,Yongyi Huang,Yiting Xu,Birong Zeng,Lizong Dai
Polyurethane is a promising topcoat in anticorrosive coating system. As a topcoat, the study on improving its weathering resistance is significative. In this work, we present an anticorrosive filler, named GOFA based on p-fluoroaniline chemical modified graphene oxide, and explored the potential of GOFA to improve the weatherability and corrosion resistance of polyurethane coatings. The results of the comprehensive experimental studies showed that the addition of 0.5 wt.% GOFA leaded to an improvement in the hydrophobicity of the polyurethane coating and the composite coating exhibits an excellent shielding effect against corrosive media. At the same time, the ultraviolet aging resistance the GOFA modified polyurethane composite coating also showed satisfactory results. It is inspired that adding a small amount of GOFA can make the composite polyurethane coating have excellent anti-corrosion performance and weather resistance.
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Inorganic Chemistry Frontiers
·
2022
·Vol. 9
·期 21
·5507-5516
·
IF 7.779
Xiaocheng Xu,Rui Wang,Sijie Chen,Alex Trukhanov,Yanxue Wu,Lianyi Shao,Le Huang,Zhipeng Sun
Developing non-noble metal-based electrocatalysts with excellent activity and stability for the hydrogen evolution reaction (HER) is crucial for the efficient electrolysis of water. Herein, self-supported three-dimensional (3D) P-doped NiSe/2H-MoSe2 nanorod arrays (denoted as P-NiSe/MoSe2) were fabricated by a hydrothermal reaction and subsequent selenization and phosphorization processes. Benefiting from P doping, the synergistic effect of the heterostructures, and abundant active sites, the P-NiSe/MoSe2 electrocatalyst exhibits excellent alkaline HER performance, with only 43 mV required to achieve 10 mA cm−2 with a Tafel slope of 93.1 mV dec−1, even remaining stable at 10 mA cm−2 for 30 hours. In addition, theoretical calculations show that the formation of the heterostructure and P doping optimize the H atom adsorption energies and accelerate electron transport, thus improving its performance in the HER. This work offers a hopeful route for the development of low-cost and efficient electrocatalysts through the simultaneous application of heterostructure engineering and heteroatom doping as well as a 3D structure.
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