Catalysts
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2022
·Vol. 12
·期 12
·1525
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IF 4.501
Sai Che,Na Ta,Fan Yang,Yulong Yang,Yongfeng Li
Rational design and construction of cost–effective electrocatalysts for efficient hydrogen production has attracted extensive research attention worldwide. Herein, we report the construction of a transition metal selenide/carbon composite catalyst featuring uniform NiSe nanoparticles anchored to single Ni atom doped porous carbon structure (NiSe/Ni–N–C) via a facile one–pot pyrolysis of low–cost solid mixtures. NiSe/Ni–N–C exhibits remarkable catalytic performance towards hydrogen evolution reaction (HER) in 1.0 M KOH, requiring a low overpotential of 146 mV to reach a current density of 10 mA cm−2. The unique carbon layer encapsulation derived from the enwrapping of fluid catalytic cracking slurry further renders NiSe/Ni–N–C excellent for long–term durability in electrolyte corrosion and nanostructure aggregation. This work paves the way for the design and synthesis of highly efficient composite HER electrocatalysts.Keywords:NiSe nanoparticle;single atom catalyst;interfacial electronic engineering;hydrogen evolution reaction
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Limin Wang,Wenhui Song,Stephen Choi,Kai Yu,Feng Zhang,Wei Guo,Yajie Ma,Kai Wang,Fengyu Qu,Huiming Lin
Sonodynamic therapy (SDT) can be described as ultrasonic (US) catalysis. Adequate charge separation is considered as effective means to promote reactive oxygen species (ROS). Here, hollow CoP@N–carbon@PEG (CPCs@PEG) nanospheres (∼60 nm) are prepared as sonosensitizers, showing greater ROS generation than pure CoP@PEG under US irradiation. Both 1O2 and ·O2– are activation species that are determined by O2 and electrons. The great SDT performance of CPCs@PEG is ascribed to the heterostructure which promotes the separation and transfer for US-generated electrons and holes. In addition, holes can be further captured by endogenous glucose that is in favor of electron aggregation and ROS generation. Moreover, the consumption of glucose would decrease intracellular ATP for starvation therapy. Given the higher oxidation ability of Co3+, CPCs@PEG nanospheres possess catalase (CAT) activity to convert H2O2 into O2 for assisting ROS generation. Moreover, they also can oxidize glutathione (GSH) as a mimic GSH oxidase to break intratumor redox balance, facilitating oxidative stress. More importantly, the nanocomposites reveal good degradation ability dominated by the oxidation from insoluble phosphide into soluble phosphate, accelerating elimination via urine and feces within 14 days. CPCs@PEG nanospheres integrate the above effects not only to reveal great tumor inhibition ability but also to excite immune activation for anticancer.
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CHEMICAL PHYSICS LETTERS
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2022
·
IF 2.719
Weiqiu Huang,Bing Zhu,Jiahui Zhu,Xufei Li,Xinya Wang,Baoyou Yan,Fei Yi,Zhen Zhang
Novel AC (termed as A-AC/SiC) with high thermal conductivity was prepared by using emulsified asphalt as precursor and polycarbosilane (PCS) as thermal conductive addition by in-situ reaction. The specific surface area and total pore volume of sample A-AC/SiC-20 was up to 1346 m 2 ·g −1 and 0.89 cm 3 ·g −1 respectively. The SEM and FIIR showed that PCS had been successfully loaded into the A-AC and formed the uniform cross-linking structure, while its thermal conductivity increased by nearly 300 % than that of the parent A-AC. Moreover, it also exhibited high adsorption capacity up to 3.46 mmol·g −1 and excellent recyclability for n-hexane vapor.
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FUEL PROCESSING TECHNOLOGY
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2022
·
IF 8.129
Linlin Liu,Mingwei Zhang,Li Wang,Xiangwen Zhang,Guozhu Li
Bifunctional catalysts with high isomerization activity and mono-branched isomer selectivity are urgently demanded for dewaxing long-chain n -alkanes. In particular, branching location of mono-branched isomer is difficult to control by current techniques. In this study, SSZ-32 zeolite with tunable distribution depth of acid sites in micropore channels is successfully prepared by ion exchange under partial template protection. Loaded with similar Pt nanoparticles , these SSZ-32 catalysts exhibit tunable activity and selectivity for hydroisomerization of n- hexadecane . Characterization results show that the adsorption model and insertion depth of n -alkane is altered by changing the distribution depth of acid sites in SSZ-32 micropore channels. When acid sites distribute in a moderate depth (∼ 4.5 nm) of the micropore channels, high yield of center-position mono-branched isomers (46.85%) is achieved, cracking reaction is significantly inhibited. The mole ratio of 6−/7−/8-methyl isomers to 2−/3-methyl isomers was increased to at least 1.3 times of the traditional catalyst with acid sites distributed throughout the micropores. The cold flow properties of lube base oils in isomerized dewaxing of Fischer-Tropsch wax are improved significantly by achieving an optimal and effective diffusion depth of reaction intermediates in the MTT micropore channels. Efficient and selective hydroisomerization of long-chain n -alkane is realized on Pt/SSZ-32 prepared by the facile partial-detemplation method.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Qian Zheng,Bingyuan Huang,Xueying Du,Juan Zhang,Hongquan Fu,Hejun Gao,Yunwen Liao
Efficient capture of radioiodine is critical during nuclear fuel reprocessing and nuclear accidents. The development of material with excellent adsorption properties of radioiodine has always been a significant challenge. Three kinds of N-loaded conjugated polymers were prepared using the solvothermal method by changing the N-group in pyrrole . The effect of nitrogen type on the structure of conjugated polymers was investigated by SEM, BET, FT-IR, XPS , and EPR. Despite their low specific surface area, their mesoporous structure is conducive to transporting iodine molecules. The results showed that in the conjugated system , the adsorption capacity of alkyl tertiary amines for iodine was better than that of aminoethyl tertiary amines and secondary amines, and the maximum adsorption capacity could reach 737.4 mg/g. The adsorption mechanism of iodine on N-loaded conjugated polymer is mainly the interaction of charge transfer between iodine and N-aromatic in the organic solution.
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ACS Applied Nano Materials
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2023
·
IF 5.9
Xiujuan Qiao,Xing-Xing Gou,Yang Li,Jian-Li Li,Tianli Yue,Qinglin Sheng,Ying-Feng Han
Gold nanoparticles (Au NPs) are often susceptible to environmental changes, especially a complexly biological environment, significantly hindering the potential application of biosensors for practical detection. However, the controllable construction of ultrastable water-soluble Au NPs for biosensing applications remains a major challenge today. Here, ultrastable water-soluble Au NPs protected by tris-N-heterocyclic carbene (NHC) ligands (2·Au NPs) have been controllably designed and synthesized. The tris-NHC shell on the Au NP surface increases the chemical and electrochemical stability of the materials, making them stable in biological environments and even in excess biomercaptan. In addition, the ammonium salt substituent on the imidazolium nitrogen not only regulates the water solubility of Au NPs but also facilitates electrostatic interactions with biological substances. Ultimately, based on the controlled synthesis of ultrastable 2·Au NPs, it is convenient to build a probe for toxic substances of ochratoxin A detection with two signal readouts. A low limit of detection (0.66 pmol·L–1) and a wide linear response range (2.5 pmol·L–1 to 25 μmol·L–1) are achieved. Meanwhile, this proposed aptasensor exhibits excellent selectivity toward various potential interfering bioanalytes and sundry ions. This work demonstrates an efficient method to regulate the properties of Au NPs by functional NHC anchors and paves the way for practical biosensing application purposes.
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POLYMER BULLETIN
·
2022
·Vol. 80
·期 10
·10825-10842
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IF 2.843
Zhang Yiqiang,Yang Fuguo,Huang Huabo,Zhao Rui,Huang Juan,Li Liang,Yu Xianghua
The multi-responsive ternary poly(N-isopropyl acrylamide) (PNIPAM)/ /sodium alginate (SA)/graphene oxide (GO) composite hydrogels were prepared. The influence of GO content on the microstructure and physical properties of the composite hydrogel was researched. The ternary composite hydrogels exhibited significantly larger mechanical strength and higher water uptake compared to binary PNIPAM/SA composite hydrogels. The effects of temperature, pH, and contact time on the adsorption capacity of rhodamine B (RB) for the PNIPAM/SA/GO ternary composite hydrogels were further investigated. The adsorption kinetic and isotherm for the adsorption behavior of the ternary composite hydrogel were well fitted with the pseudo-second-order kinetic model and Langmuir model, respectively. Besides, the PNIPAM/SA/GO ternary composite hydrogel could be easily removed from the dye solutions and reused without the obvious decrease of its performance. It indicated that the ternary composite hydrogel could serve as an effective adsorbent for the removal of organic pollutants.
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Journal of Energy Chemistry
·
2023
·
IF 13.1
Yonghai Feng,Min Yu,Minjia Meng,Lei Liu,Dewei Rao
In the selective oxidation of biomass-based 1,2-propanediol (PDO) with oxygen as the terminal oxidant, it is challenging to improve the lactic acid (LA) selectivity for nonnoble metal nanoparticles (NPs) due to their limited oxygen reduction rate and easy C–C cleavage. Given the high economic feasibility of nonnoble metals, i.e., Cu, in this work, copper and nitrogen codoped porous carbon nanosheets encapsulating ultrafine Cu nanoparticles (Cu@Cu-N-C) were developed to realize highly selective of PDO oxidation to LA. The carbon-encapsulated ultrasmall Cu 0 NPs in Cu@Cu-N-C have high PDO dehydrogenation activity while N-coordinated Cu (Cu-N) sites are responsible for the high oxygen reduction efficacy. Therefore, the performance of catalytic PDO conversion to LA is optimized by a proposed pathway of PDO → hydroxylacetone → lactaldehyde → LA. Specifically, the enhanced LA selectivity is 88.5%, and the PDO conversion is up to 75.1% in an O 2 -pressurized reaction system (1.0 MPa O 2 ), superior to other Cu-based catalysts, while in a milder nonpressurized system (O 2 flow rate of 100 mL min −1 ), a remarkable LA selectivity (94.2%) is obtained with 39.8% PDO conversion, 2.2 times higher than that of supported Au nanoparticles (1% Au/C). Moreover, carbon encapsulation offers Cu@Cu-N-C with strong leaching resistance for better recycling.
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BIOPROCESS AND BIOSYSTEMS ENGINEERING
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2023
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IF 3.8
Zhong Linhan,Chen Ye,Wen Qing,Yang Yang
The focus of this study is to develop a high-performance anode material for microbial fuel cells (MFCs). PEDOT:PSS and nitrogen-modified MXene were combined to create a hydrogel composite material called PPNM, which was drop-cast onto carbon felt (CF) as the MFCs anode. The PPNM exhibited a higher peak power density of 4.78 W m −2 , an increase of 332% compared to the CF anode. It is worth noting that the PPNM Hydrogel maintains its rough and porous structure, providing favorable sites for bacterial colonization. The introduction of N-MXene has improved the electrochemical performance of the hydrogel, particularly impacting the mediated electron transfer process. Microbial community analysis revealed the presence of more electrochemically active species on the PPNM anode. These findings highlight the potential of PPNM hydrogel and pave the way for similar strategies in achieving high-performance anodes in MFCs.
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ACS ES&T Water
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2023
·
IF 5.3
Peizeng Yang,Jiayue Dong,Haiyan Wang,Teng Zhang,Gregory V. Korshin,Junhe Lu
N-Nitrosodimethylamine (NDMA) is a disinfection byproduct and a probable human carcinogen formed during water treatment processes. While its generation in engineered systems has been extensively explored, its formation in natural environments is inadequately understood. This study demonstrates that compounds with dimethylamine (DMA) functionality exposed to sunlight irradiation in the presence of nitrite (NO2–) react to form NDMA. The molar yields of NDMA ranged from 0.006 to 0.035% after 6 h irradiation. The radicals generated by the photolysis of NO2–, notably •OH, NO•, and NO2•, play critical roles in this process. Three reaction pathways are involved in the NDMA formation. In the first and second pathways, nitrogen oxide radicals couple or dimerize to form the nitrosating agents N2O3 and N2O4, which attack the DMA moiety, yielding NDMA. In the third pathway, the DMA moiety is oxidized by •OH via H-abstraction to produce a nitrogen-centered radical (CH3N•CH3) which, followed by the addition of a NO•, yields NDMA. Radical quenching experiments combined with theoretical calculations suggest that the •OH/H-abstraction pathway is more favorable. Given that many environmental contaminants contain DMA functionalities, the photochemical formation pathway of NDMA in the sunlit surface waters may be important for aquatic environments.
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Polymer Chemistry
·
2023
·Vol. 15
·期 2
·97-105
·
IF 4.6
Donghui Zhang,Shiqi Liu,Zhihao Cai,Weizhe Luo,Guojian Liu,Runhui Liu
Polypeptides are extensively used in the fields of biomedicine and biomaterials. The use of N-phenoxycarbonyl amino acids (NPCs) as monomers for polypeptide synthesis is an advanced method that offers the unique advantage of excellent monomer stability. However, the purification of NPC monomers previously required laborious column chromatography or recrystallization techniques, which might have restricted the widespread application of NPC polymerization. In this work, a straightforward and efficient method for synthesizing NPC monomers has been developed, enabling the production of products with high purity through a simple work-up process. This method is compatible with various amino acids, and the resulting monomers can undergo normal polymerization reactions. By significantly enhancing the availability of NPC monomers, this method facilitates the synthesis of polypeptides.
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Advanced Electronic Materials
·
2023
·Vol. 10
·期 3
·2300651
·
IF 6.2
Tianpeng Yu,Shuyi Hou,Zhenliang Liu,Yiru Wang,Jiang Yin,Xu Gao,Nannan Liu,Guoliang Yuan,Lei Wu,Yidong Xia,Zhiguo Liu
Organic field-effect transistors (OFETs) hold great promise for applications in non-volatile memories, detectors, and artificial synapses due to the good flexibility and biocompatibility. However, certain drawbacks such as high operating voltages and significant degradation in endurance characteristics have hindered their practical implementations. Herein, a novel approach is proposed to enhance the performance of OFETs by incorporating a bi-functional n-type polymer semiconductor interlayer, Poly-{[N,N'-bis(2-octyldodecyl)naphthalene-1,4,5,8-bis(dicarboximide)-2,6-diyl]-alt-5,5′-(2,2′-bithiophene)} (N2200), into a pentacene OFET structure. The device exhibits remarkable improvements, with reliable P/E operation cycles of over than 10 4 and a retention time of more than 10 years. On one hand, the inclusion of N2200 as an n-type semiconductor effectively reduces the height of hole-injection barrier for trapping and thus reducing the working voltage based on the electrostatic induction theory. On the other hand, n-type semiconductor N2200 serves as a native hole-consumption (or hole-trapping) dielectric, and its narrower bandgap restrains the formation of deep hole-traps, thus favoring the endurance characteristics of the OFET.
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