RSC Advances
·
2023
·Vol. 13
·期 41
·28931-28939
·
IF 3.9
Guoqing Li,Zhiyi Zhang,Wenhao Xiao,Tongtong Wu,Jinbao Xu
The broad application of polyacrylamides (PAMs) has greatly promoted the development of new synthetic methods to prepare PAM-based functional (co)polymers regarding their traditional preparation via the direct polymerization of various acrylamide monomers. Herein, we have explored the post-polymerization modification of the poly(2,2,2-trifluoroethyl acrylate) (PTFEA) homopolymer, a typical non-activated ester, and various amines using the organo-catalytic system involving 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU) and 1,2,4-triazole (TA). The reaction kinetics (e.g., the optimized reaction solvent, temperature, time, initial molar ratio of amines to esters and the molar ratio of DBU to TA) were carefully studied with the modulus substrate of iso-propylamine as the formed poly(iso-propyl acrylamide) (PNIPAM) representing the most investigated PAM. The full and partial amidation of the esters in PTFEA could be precisely regulated just by controlling the kinetic conditions to give (co)polymers with designable compositions and structures. We have demonstrated that the poly(N-acryloyl pyrrolidine) obtained by the post-polymerization modification of non-activated ester and pyrrolidine exhibited a noticeable phase transition, which confirmed the robustness and versatility of the post-polymerization modification. The described method paves the way for the synthesis of various (co)polymers with amide side chains from readily available polymer precursors.
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Xian Zhang,Cheng-Ye Zhu,Wangbei Cao,Zhao-Yu Ma,Hao-Nan Li,Hong-Qing Liang,Chuan-Jie Fang,Xiao-Jun Huang,Zhi-Kang Xu
Poly(propylene-co-1-butene) (PP-co-BT) is a promising material for membrane separation, due to its greater flexibility, reduced melting point and lower crystallinity relative to other polyolefins including polypropylene and poly(4-methyl-1-pentene). Nevertheless, employing PP-co-BT in membrane separation poses a challenge due to the limited understanding of its thermodynamic and kinetic behavior in solution, as well as the lack of the appropriate means of optimizing membrane morphologies for specific applications. In this study, we aim to address these challenges by reporting the preparation of PP-co-BT membranes via the thermally induced phase separation (TIPS) process using soybean oil and dibutyl phthalate as mixed diluent. The thermodynamic phase diagram demonstrates a liquid–liquid phase separation mechanism. By employing an isotropic cooling condition, we fabricate symmetric membranes with uniformly distributed bi-continuous pores. These membranes are subsequently coated with a mussel-inspired coating to achieve Janus wettability, enabling efficient separation of oil-in-water emulsions. Furthermore, we demonstrate the ability to produce PP-co-BT membranes with gradient or asymmetric porous structures by subjecting the TIPS process to temperature or concentration gradients. These gradient or asymmetric membranes hold promise for specific applications such as the removal of microplastics from water or as oxygenation membranes. This study showcases the potential of PP-co-BT in membrane separation, offering insights into the fabrication techniques and the versatility of PP-co-BT for various applications.
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Journal of Energy Chemistry
·
2023
·
IF 13.1
Qingchun Zhang,Di Liu,Yaping Zhang,Zhiliang Guo,Minpeng Chen,Yuyun Chen,Bo Jin,Yingze Song,Hui Pan
The development of highly active, selective, and stable electrocatalysts can facilitate the effective implementation of electrocatalytic CO 2 conversion into fuels or chemicals for mitigating the energy crisis and climate problems. Therefore, it is necessary to achieve the goal through reasonable material design based on the actuality of the operational active site at the molecular scale. Inspired by the stimulating synergistic effect of coupled heteronuclear metal atoms, a novel Ni-Co atomic pairs configuration (denoted as NiN 3 ©CoN 3 -NC) active site was theoretically screened out for improving electrochemical CO 2 reduction reaction (CO 2 RR). The structure of NiN 3 ©CoN 3 -NC was finely regulated by adjusting Zn content in the precursors Zn/Co/Ni-zeolite imidazolate frameworks (Zn/Co/Ni-ZIFs) and pyrolysis temperature. The structural features of NiN 3 ©CoN 3 -NC were systematically confirmed by aberration-corrected HAADF-STEM coupled with 3D atom-overlapping Gaussian-function fitting mapping, XAFS, and XRD. The results of theoretical calculations reveal that the synergistic effect of Ni-Co atomic pairs can effectively promote the *COOH intermediate formation and thus the overall CO 2 RR kinetic was improved, and also restrained the competitive hydrogen evolution reaction. Due to the attributes of Ni-Co atomic pairs configuration, the developed NiN 3 ©CoN 3 -NC with superior catalytic activity, selectivity, and durability, with a high turnover frequency of 2265 h −1 at −1.1 V (vs . RHE) and maximum Faradaic efficiency of 97.7% for CO production. This work demonstrates the great potential of DACs as highly efficient catalysts for CO 2 RR, provides a useful strategy to design heteronuclear DACs, exploits the synergistic effect of multiple metal sites to facilitate complex CO 2 RR catalytic reactions, and inspires more efforts to develop the potential of DACs in various fields.
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Journal of Energy Storage
·
2023
·
IF 9.4
Haonan Zhang,Lin Fang,Yuanchao Guo,Zhongzhu Wang,Haibo Hu,Wen He,Peihong Wang
Supercapacitors (SCs) have attracted extensive attention due to the properties of high power density, long cycle life, and high rate performance. However, the high self-discharge is one giant challenge for long-term energy storage applications of SC. Herein, we prepared a high-performance SC with low self-discharge based on nitrogen-sulfur co-doped ZIF-8-derived (NS-PC) materials. The synergistic effects of high-temperature carbonization and nitrogen-sulfur (N-S) doping are systematically investigated. With a carbonization temperature of 900 °C, assisted with N-S doping, the maximum specific capacitance of the NS-PC-900//NS-PC-900 symmetrical SC is 42.7 F g −1 , while the power densities range from 650 to 13,000 W kg −1 at the energy densities of 10.04–7.5 Wh kg −1 . The specific capacitance remains 95.7 % even after 20,000 charge-discharge cycles. More importantly, the as-prepared NS-PC-900//NS-PC-900 SC exhibits an ultra-low self-discharge rate of solely 0.025 V h −1 within 24 h. This work provides a universal strategy to fabricate high-performance SCs with low self-discharge.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Bin Liu,Xinyu Wang,Rongyue Wang,Guanyi Zhang,Xiaoqin Xu,Jin Liu,Zhiyao Sun,Mingyang Liu,Cheng Wang,Xin Meng,Jiahao Xie,Jinlong Zou
Catalysts with high activity and corrosion-resistance are desirable for oxygen reduction and evolution reactions (ORR/OER) in rechargeable zinc-air batteries (ZABs). Herein, via an etching-phosphating-annealing strategy, CoP is in situ formed in hollow carbon-nanobox, both of which are wrapped by a thin nitrogen-doped carbon layer (CoP/HNBs@NCL). Tannic acid etches ZIF-67 nanobox to release Co 2+ and 2-methylimidazole to generate hollow structure. As-marked CoP/HNBs@NCL-2 (271.9 m 2 g −1 ) exhibits robust activities towards ORR (half-wave potential of 0.88 V) and OER (overpotential of 0.36 V), which outperforms many non-precious metal catalysts due to the strong interactions between CoP and N-species and the smooth mass transfer via the porous hollow structure. Even at high potentials (OER), HNBs@NCL framework can still relieve the leaching of Co species (leaching ratio of 15.5 % after 6 h) to obtain high corrosion resistance and stability. Theoretical calculations reveal that N atoms enhance the electron delocalization degree of Co sites in CoP to lower energy barriers and balance adsorption free-energies of O-intermediates to enhance oxygen electrocatalysis. Notably, ZAB with CoP/HNBs@NCL-2 air-electrode exhibits high peak power density (139.8 mW cm −2 ) and charge–discharge cycling stability (132 h). This work presents a reliable protocol to design hollow electrocatalysts with desirable bifunctional activity and stability for ZABs.
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CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Ye Zhaochun,Yao JiaCheng,Zheng Wen,Yuan Wenhui,Guan Jianyu,Li Li,Xiao Hong
Octafluoropropane (C 3 F 8 ) is a kind of super greenhouse gas, and the low concentration of octafluoropropane makes it difficult to be adsorbed and removed. In this study, a series of Co-doped MOFs (Co x Cr-MIL-101) have been successfully synthesized using a hydrothermal method without the addition of strong acids such as HF. The structural properties of the prepared Co x Cr-MIL-101 are characterized using SEM, XRD, nitrogen adsorption desorption test, etc. The adsorption properties of C 3 F 8 are measured by single-component isothermal adsorption experiments and fixed bed adsorption breakthrough experiments. The adsorption mechanism was investigated via the adsorption theory models. The results show that the introduction of cobalt ions can effectively improve the adsorption capacity of MIL-101, among which the Co 0.2 Cr-MIL-101 exhibits the best adsorption performance. The C 3 F 8 equilibrium adsorption capacity reaches 0.077 mmol/g at 298 K and 180 Pa, which is 3.03 times that of the pristine MIL-101 and the dynamic adsorption capacity is 20.710 mmol/g (298 K, 1.2 L/min), which is 9.37 times that of the pristine MIL-101. Inspiringly, the IAST separation selectivity of C 3 F 8 /N 2 at 100 kPa is up to 146.7, which is 14.3 times that of the pristine MIL-101. More importantly, the co-modified adsorbent showed better thermal stability and cyclic stability. In addition, Co 0.2 Cr-MIL-101 fits the Freundlich isothermal adsorption model, and the adsorption mechanism analysis shows that the high adsorption capacity of Co 0.2 Cr-MIL-101 benefits from the unique pore structure and abundant active sites of the modified MOFs.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Can Fang,Xiangmei Tang,Qingfeng Yi
Exploring efficient non-precious metal oxygen electrocatalysts for oxygen reduction/evolution reactions (ORR/OER) is of great importance in electrochemical energy conversion devices like metal-air battery. Among them, carbon-based composites derived from metal-organic framework (MOF) exhibit excellent catalytic performance in ORR/OER. In this paper, Co-MOF-67 was firstly prepared, and then mixed with FeCl 3 ·6 H 2 O and dicyandiamide, followed by a one-step pyrolysis to obtain bamboo-like nitrogen-doped carbon nanotubes . For the samples, Fe and Co nanoparticles were encapsulated in the front end of the carbon nanotubes and the presence of new (n)-diamond carbon was unexpectedly found. The obtained catalyst (FeCo@CNTs-60) has an onset potential of 1.04 V for ORR in alkaline solution, which is close to the commercial Pt/C (40 wt% Pt) of 1.05 V. The onset potential of 1.02 V in quasi-neutral solution exceeds that of Pt/C of 0.99 V. In addition, FeCo@CNTs-60 exhibited a low potential difference of 0.81 V between OER and ORR potentials. The alkaline zinc-air batteries, fabricated with the sample as the electrocatalyst of air electrode, exhibit higher peak power density and stability than Pt/C, while the rechargeable batteries present superior cycling discharge/charge stability at 5 mA·cm −2 and 10 mA·cm −2 . In particular, the battery with FeCo@CNTs-60 was conducted for continuous over 1300 h of ultra long-term cycle charging / discharging test at a current density of 5 mA·cm −2 , and it reveals excellent stability with high voltage efficiency and also presents superior cycle charging / discharging stability after replacing the Zn plates and electrolyte.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Haixiang Lv,Xuchao Li,Jiaqing Li,Chang Yu,Qinghong Zeng,Guogui Ning,Hu Wan,Jianhong Li,Kangsheng Ma,Shun He
The cotton aphid Aphis gossypii Glover (Homoptera: Aphididae) is a notorious agricultural pest that has evolved high levels of resistance to various insecticides. Innovative RNA insecticides, as potential green plant protection products, are anticipated to alleviate the significant issue of pest resistance. Herein, a rough-surface hollow mesoporous silica (RHMS)-based gene/insecticide delivery system was constructed for the co-delivery of CYP6CY13 double-stranded RNA (dsRNA) and the chemical insecticide imidacloprid for the effective control of A. gossypii . The hollow mesoporous structure of RHMS facilitates insecticide loading and further combines with dsRNA through electrostatic interactions to form nanoscale complexes, while protecting the dsRNA from complete degradation by nucleases. The screened ds CYP6CY13 fragment was successfully expressed in the L4440-HT1115 (DE3) RNaseIII - system and inhibiting CYP6CY13 expression by RNA interference (RNAi) significantly increased the susceptibility of A. gossypii adults to imidacloprid. The toxicity of the RHMS/IMI/ds CYP6CY13 complex was significantly higher (1.95-fold) than that of imidacloprid. The results of the pot test showed that the effectiveness of the RHMS/IMI/ds CYP6CY13 complex against A. gossypii improved by 19.95 % in 5 days. Therefore, this nanoparticle-mediated gene/insecticide co-delivery system is expected to be an effective tool for pest control.
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ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Guilian Li,Minqiao Lu,Fan Wang,Yueteng Hou
Microbial fuel cells (MFCs) are being recognized as a promising solution for sustainable energy generation and wastewater treatment . Despite their potential, MFCs face certain challenges that must be overcome, such as the problem of low power output caused by inefficient extracellular electron transfer (EET). In this study, we develop a nanoporous CoC x /Co@CC composite anode using microwave-assisted and high-temperature calcination methods to enhance EET efficiency and bacterial adhesion in MFCs. Compared with pure carbon cloth (CC) anodes, MFCs with CoC x /Co@CC anodes exhibit a 1.24-fold increase in power density, with a maximum output of 2693 mW m −2 . The improved performance can be attributed to the lower charge transfer resistance (R ct ) and higher redox activity of the CoC x /Co@CC anode. Cobalt's multiple valence states enhance its ability to transfer electrons between microorganisms and electrodes, ultimately increasing the overall redox activity. The CoC x /Co@CC anode also promotes the growth and enrichment of exoelectrogens, with Geobacter being enriched up to 75 % at the anode, compared with 46 % at the CC electrode. These findings demonstrate the potential of CoC x /Co@CC anodes for improving the EET efficiency of MFCs, which can have significant implications for sustainable energy and wastewater treatment.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2023
·
IF 4.4
Xuan Liu,Xiaojia Su,Zhuohang Ren,Lingqiu Yang,Xinyue Zhang,Mingye Ding
Currently, developing advanced optoelectronic materials is of great importance to solving serious problem of fake and shoddy products. Lanthanide-doped nanomaterials are particularly suitable for addressing this issue, but limited by the realization of multiple upconverison (UC) emissions upon a single-wavelength laser excitation. Herein, it is proven that the co-dopant of blue/near-infrared (NIR)-emitting activators (Tm 3+ ) and green/red-emitting centers (Er 3+ ) in a particular designed core–shell nanoarchitecture allows the achievement of multiple luminescence over wide spectral region for optical security. In our study, cubic-phased NaYbF 4 :Tm/Er@CaF 2 nanocrystals have been successfully synthesized through a layer-by-layer coprecipitation strategy, which presents visible multicolor UC luminescence and invisible NIR UC emission upon 980 nm laser excitation by just regulating the laser power and temperature. Significantly, the unique luminescent characteristics enables the designed UC nanoparticles a promising candidate for advanced anti-counterfeiting. This works offers a reference to develop advanced optoelectronic materials for practical application in optical security.
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2023
·
IF 8.4
Jiajing Xu,Weiqiang Yang,Jiancong Ni,Qingxiang Wang,Zhenyu Lin
Electrochemiluminescence (ECL) arises from the collisional annihilation between the electro-excited luminophore and co-reactant. Most ECL-based bioassays require extensive free co-reactants that collide with luminophores randomly. Herein, the N,N-dimethylaniline (DMA) group was electro-grafted on the ITO electrode surface as the bottom co-reactant layer, and the vertically ordered mesoporous silica film (VMSF) was prepared as the upper layer to regulate the accessibility of Ru(bpy) 3 2+ . Thus, the dual-layer functionalized VMSF/N-ITO was newly built for the controllable ECL study. Relevant conditions, including the DMA electro-grafting, VMSF thickness, buffer concentration and pH value, were discussed to improve the ECL efficiency. Based on the VMSF/N-ITO platform, a homogeneous ECL bioassay was developed for miRNA-21 detection. The target nucleotide sequence induced the hybridization chain reaction (HCR) of probes H1 and H2 to absorb free Ru(bpy) 3 2+ as much as possible. Residual Ru(bpy) 3 2+ permeated the VMSF nanochannels to collide with the DMA co-reactant in producing an ECL response. There was a linear relationship between ∆ECL intensity and logarithmic concentration of miRNA-21 in the 1 fM ∼ 100 pM range, and the detection limit was 0.25 fM. The developed approach was probes immobilization-free, highly sensitive, and anti-interference, opening a new avenue for ECL-based bioassays.
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NANOTECHNOLOGY
·
2023
·Vol. 35
·期 11
·115203
·
IF 3.5
Qingyong Qin,Yu Liu,Ge Gao,Zhaoqiong Chen,Zejiang Gao,Li Chen,Xianci Zhong,Bingsuo Zou
Lead-free halide double perovskites are considered as one of the most promising materials in optoelectronic devices, such as solar cells, photodetectors, and light-emitting diodes (LEDs), due to their environmental friendliness and chemical stability. However, the extremely low photoluminescence quantum yield (PLQY) of self-trapped excitons (STEs) emission from lead-free halide double perovskites impedes their applications. Herein, Sb3+ ions were doped into rare-earth-based double perovskite Cs2NaScCl6 single crystals (SCs), resulting in a large enhancement of PLQY from 12.57% to 87.37%. Moreover, by co-doping Sb3+ and Ho3+ into Cs2NaScCl6 SCs, the emission color can be tuned from blue to red, due to an efficient energy transfer from STEs to Ho3+ ions. Finally, the synthesized sample was used in multicolor LED, which exhibited excellent stability and optical properties. This work not only provides a new strategy for improving the optical properties of Cs2NaScCl6 SCs, but also suggests its potential application in multicolor LEDs.
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