NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 45
·21730-21736
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IF 3.925
Ziyue Zhou,Renjiang Li,Ke Li,Kai Zong,Dongshun Deng
The efficient capture and separation of ammonia (NH3), a fundamental raw material as well as widespread pollutant, is significant in the fertilizer industry and for environmental protection protocols. In this work, several new type V deep eutectic solvents (DESs), composed of hydroxypyridine and phenol, were designed as efficient and reversible NH3 absorbents. All the DESs have low viscosity, good NH3 absorption performance and high NH3/CO2 selectivity. The optimal 3-hydroxypyridine/phenol (1 : 5) ratio could respectively capture 10.00 mol kg−1 and 4.63 mol kg−1 NH3 at pressures of 101.3 kPa and 10.0 kPa, better than most other DESs and ILs reported in the literature. The prepared DESs show satisfactory thermal stability and highly reversible absorption performance. By comprehensively analyzing the absorption behavior and spectroscopic results, the effective NH3 absorption ability of DESs was deduced being due to a relatively strong interaction between multiple weak acidic hydroxyl groups and basic NH3.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Zhe Li,Jizhao Zou,Tao Liang,Xinrui Song,Zhangjian Li,Jiaming Wen,Minggui Peng,Xierong Zeng,Haitao Huang,Hongliang Wu
Developing heterostructures in nano-electrocatalyst has been demonstrated as a feasible method to enhance electrocatalytic activities for water splitting, since it still remains a grand challenge to develop highly efficient and stable electrocatalysts for both oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) within a wide pH range. Herein, we report a facile pyrolysis strategy of Ru-MOF for rationally constructing ultrasmall Ru@RuO 2 heterostructures, which exhibit extremely remarkable electrocatalytic performance toward both HER and OER in pH-universal electrolytes. Impressively, optimal Ru@RuO 2 -250 achieves ultralow overpotentials for both OER (198 mV, 263 mV and 182 mV @ 10 mA cm −2 in acidic, neutral and alkaline media) and HER (31 mV, 43 mV and 32 mV @ 10 mA cm −2 in acidic, neutral and alkaline media) due to the full exposure of highly active sites, which are derived from the synergism of abundant heterointerfaces, ultrafine heterostructure size and hierarchical porous structure with high surface area. Theoretical calculations reveal the charge rearrangement and electron conduction intensification near Ru-RuO 2 heterointerfaces, the electronic structure changes of the active sites optimize the adsorption behavior toward various reaction intermediates, reducing the activation barriers and speeding up the reaction kinetics. Deservedly, an asymmetric-electrolyte electrolyzer employed with Ru@RuO 2 -250 is assembled to acquire an ultralow applied voltage of 0.79 V at 10 mA cm −2 based on amphoteric water electrolysis (HER in acidic electrolyte while OER in alkaline electrolyte).
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
·
IF 7.139
Lan Wang,Ning Gong,Zhou Zhou,Wenchao Peng,Yang Li,Fengbao Zhang,Xiaobin Fan
Developing highly efficient, durable and noble-metal-free electrocatalysts for hydrogen evolution reaction (HER) in a wide pH range is the key to achieve sustainable energy cycle. Modulating the electronic characteristics of catalysts is of great important to enhance their electrocatalytic performance. Herein, we successfully design a self-supported multi-element transition metal phosphide (V-CoP/Ni 2 P/NF) electrocatalyst by V-doping and interface engineering. According to DFT calculations, V dopants and the synergistic effect between CoP and Ni 2 P can bring optimal hydrogen/water adsorption free energies . Meanwhile, the 3D cross-linked network structure could expose abundant active sites and facilitate ions diffusion/electron transfer. As a result, the V-CoP/Ni 2 P/NF catalysts exhibit superior electrocatalytic activities with extremely low overpotentials of 20, 58 and 79 mV to deliver a current density of 10 mA cm −2 for HER in alkaline, neutral and acidic electrolytes, respectively. Moreover, they also display outstanding long-term stability. This electronic modulation strategy provides a promising pathway for energy-related catalysis processes.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2022
·
IF 3.898
Da Ke,Minjia Wang,Jiancheng Ruan,Xinzhi Chen,Shaodong Zhou
Continuous preparation of pyromellitic dianhydride (PMDA) from durene has been studied using a fixed-bed reactor. The reaction was performed using a phosphorus-vanadium-titanium ternary catalyst. Relatively high selectivity and yield of PMDA was obtained. The in-situ characterization was combined with theoretical calculation to reveal the reaction mechanisms, and the remarkable doping effect was discussed.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Baojie Zhang,Changti Pan,Hengjie Liu,Xingshun Wu,Hongliang Jiang,Li Yang,Zeming Qi,Guang Li,Lei Shan,Yunxiang Lin,Li Song,Yong Jiang
Urea oxidation reaction (UOR) has emerged as a competitive approach for many energy-related technologies due to the low overpotential and fast reaction dynamics. The main challenge lies in fabricating high-efficient catalysts with optimized electronic structure and understanding the intrinsic structure-related mechanisms. Here, we report a feasible strategy of regulating the rate-determining step (RDS) of UOR via an electrochemical reconstructed Co hydroxide catalyst incorporated with V single atoms. The optimal catalysts exhibit an enhanced UOR performance after V incorporation while remarkably suppressed the competitive oxygen evolution with the potential of 1.54 V (vs RHE) to achieve the current density of 30 mA cm −2 . Operando synchrotron-radiation Fourier transform infrared spectroscopy (SR-FTIR) combining density functional theory (DFT) calculations reveal that enabled by single atom V incorporation, the RDS of UOR has been changed from the first deprotonation step to the second one with a lower energy barrier of 2.05 eV (vs 2.6 eV), which is thermodynamically favorable for the overall reaction process.
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JOURNAL OF POWER SOURCES
·
2022
·
IF 9.794
Yani Liu,Yu Wang,Haoqiang Wang,Shuming Dou,Junwei Wu,Wei Gan,Qunhui Yuan
Aiming to the repetitively large volume change and the inevitably loss of volumetric capacity of bismuth (Bi) based sodium-ion battery (SIB) during cycling, a binder-free Bi anode based on one-step electrochemical co-deposited three-dimensional Bi nanosheets and conductive carbon nanotube networks (Bi NS/CNTs) was developed. Compared with the sole Bi anode achieved via the same strategy, the co-deposition of 3D hierarchical Bi nanosheet/CNTs arrays manifests the strong interfacial adhesion and accommodates the volume change upon sodium alloying/dealloying. Such structural feature endows the Bi NS/CNTs anode a long-term cycling stability (383.72 mAh g −1 at 0.1 A g −1 after 200 cycles, 311.68 mAh g −1 at 1 A g −1 after 1000 cycles) and a good rate performance. A full SIB assembled with Bi NS/CNTs anode and Na 3 (VOPO 4 ) 2 F@rGO cathode shows a high operating voltage (above 4 V) and a high energy density of 221.99 Wh kg −1 , which outperforms many reported Bi-based analogues. This work may open a new opportunity for developing efficient SIB with high energy and good practicability.
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JOURNAL OF MATERIALS SCIENCE
·
2021
·Vol. 56
·期 31
·17694-17708
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IF 4.22
Bu Jingting,Zhou Zhipeng,Wu Xiaomin,Zhang Chenying,Li Zhen
Biomass-derived carbon materials are often applied in green energy storage systems like supercapacitors due to the abundance, facile access, low cost and nontoxicity. In this work, biomass-derived porous carbon spheres (PCSs) have been prepared by the carbonization and etching of sodium alginate (SA). Using polyacrylic acid (PAA) as a template, N-doped graphene quantum dots (N-GQDs) are grown evenly on the surface of the PCSs, which drastically improves the pseudocapacitive activity and electrical conductivity. The prepared N-GQD/PCS/PAA electrode has a remarkable specific capacitance of 419.3 F g −1 at 1 A g −1 . The symmetric supercapacitor assembled with N-GQD/PCS/PAA electrode exhibits a great specific capacitance of 337.5 F g −1 at 0.5 A g −1 . Particularly, the device displays an ultrafast charge/discharge rate of 2.5 V s −1 , demonstrating excellent rate capability and structural stability. The supercapacitor based on N-GQD/PCS/PAA possesses high energy density of 11.72 W h kg −1 and excellent cycle stability. A high mass loading (9.18 mg cm −2 ) with the energy density of 8.54 W h kg −1 is also investigated to realize the practical application for the device. In general, a novel biomass-derived carbon electrode modified with highly electrochemical active N-doped graphene quantum dots has been constructed to provide an effective way for high performance energy storage.
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ACS Omega
·
2021
·
IF 3.512
Ruiming Xiao,Wanci Liao,Guangjuan Luo,Zhenning Qin,Shuangyan Han,Ying Lin
Mogroside V (MV), a sweetener, is one of the major components inSiraitia grosvenorii. In our research, after in vitro incubation with MV for 24 h, the human gut microbiota diversity changed, with an enrichment of the genera Bacteroides, Lactobacillus, Prevotella, Megasphaera, and Olsenella and the inhibition of Clostridium XlVa, Dorea, and Desulfovibrio. Moreover, the synthesis of short-chain fatty acids, such as acetate, propionate, and butyrate, was increased by gut microbiota. According to ultraperformance liquid chromatography–mass spectrometry (UPLC-MS) analysis, MV was decomposed into secondary mogrosides, such as mogroside II/I and mogrol, by gut microbiota. Enhanced antioxidant abilities of the metabolites were found in the broth. The results suggested that MV, as a potential prebiotic, could benefit human health through its interaction with gut microbiota.
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Shifeng Zhao,Zhaosong Li,Haiyan Wang,Hanhan Huang,Caifeng Xia,Derui Liang,Junshan Yang,Qian Zhang,Zilin Meng
Mg-Al layered double hydroxides coated waste textile (MgAl-LDH@WT) was prepared by an in-suit method for the separation of toxic metal ions such as As(V) and Cr(VI) from soil samples. Kinetics studies of As(V)/Cr(VI) removal by MgAl-LDH@WT with different Mg/Al ratio were well described by intraparticle diffusion and pseudo-second-order model. Adsorption isotherm data of As(V)/Cr(VI) yielded a better accordance of Langmuir model, manifesting that accessible adsorption site was the main influence factor and the removal of As(V)/Cr(VI) was a charge-limited process. The adsorption capacity was 69.8 mg/g, 49.8 mg/g, 45.6 mg/g and 38.2 mg/g by Mg 2 Al-LDH@WT, Mg 3 Al-LDH@WT, Mg 4 Al-LDH@WT and LDHs, and for Cr(VI) were 27.5 mg/g, 24.9 mg/g, 19 mg/g and 6.8 mg/g, respectively. Adsorption behavior of As(V) and Cr(VI) co-existing in soil indicated that As(V) possess a preferential adsorption rather than Cr(VI) by Mg 2 Al-LDH@WT, and molecular simulation was selected to explain the results of competitive relationship by bonding energy and variation of bond length. The effect of co-existing ions, column leaching experiment and recycle experiment for practical performance assessment were also examined, and these results revealed a high stability and a good partition capability. The performance of excellent removal and convenient recovery suggested a promising strategy in anionic heavy metals contaminated soil.
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Small
·
2020
·Vol. 16
·期 13
·1907163
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IF 11.459
Rongxiang Hu,Huayu Qiu,Huanrui Zhang,Peng Wang,Xiaofan Du,Jun Ma,Tianyuan Wu,Chenglong Lu,Xinhong Zhou,Guanglei Cui
Lithium (Li) metal batteries (LMBs) are enjoying a renaissance due to the high energy densities. However, they still suffer from the problem of uncontrollable Li dendrite and pulverization caused by continuous cracking of solid electrolyte interphase (SEI) layers. To address these issues, developing spontaneously built robust polymer-reinforced SEI layers during electrochemical conditioning can be a simple yet effective solution. Herein, a robust homopolymer of cyclic carbonate urethane methacrylate is presented as the polymer matrix through an in situ polymerization method, in which cyclic carbonate units can participate in building a stable polymer-integrated SEI layer during cycling. The as-investigated gel polymer electrolyte (GPE) assembled LiCoO 2 /Li metal batteries exhibit a fantastic cyclability with a capacity retention of 92% after 200 cycles at 0.5 C (1 C = 180 mAh g −1 ), evidently exceeding that of the counterpart using liquid electrolytes. It is noted that the anionic ring-opening polymerization of the cyclic carbonate units on the polymer close to the Li metal anodes enables a mechanically reinforced SEI layer, thus rendering excellent compatibility with Li anodes. The in situ formed polymer-reinforced SEI layers afford a splendid strategy for developing high voltage resistant GPEs compatible with Li metal anodes toward high energy LMBs.
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PubMed
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ACS Applied Nano Materials
·
2019
·
IF 0
Jiaxing Wei,Mohamed F. Aly Aboud,Imran Shakir,Zhangfa Tong,Yuxi Xu
The application of sorbent in solving the water pollution induced by heavy metals or metalloids is severely hindered by poor sorption performance and high cost, especially in simultaneous removal. Design and synthesis of nanocomposites as effective sorbents has been widely considered as a promising approach to address this problem. Herein, graphene oxide supported organo-montmorillonite composite (GO-OM) was prepared through a facile ultrasonic-assisted method for the first time and exhibited excellent synergetic adsorption behavior for mixed pollutants in aqueous solutions. Unlike previous studies, the simultaneous removal process can be well-described by the Freundlich and pseudo-second-order kinetic models. The sorption capacities of GO-OM are very high for both metal cations and oxyanionic groups, showing excellent potential in the removal of multiple contaminants. Our study also reveals that GO-OM has high recycling efficiency and good performance under a low level concentration. All results suggest that GO-OM can be used as effective and ecofriendly sorbents for the removal of combined pollutants in an aqueous environment. This work contributes to developing high-performance graphene materials with organic minerals and gives deep insight into simultaneous sorption of metal ions, which can be potentially extended to other multiple pollutants.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Zibin Pan,Zhengxian Chen,Gary Owens,Zuliang Chen
Biosynthesis strategies are promising methods for the sustainable preparation of nanoparticles because they are less toxic to living organisms and the environment. However, there are still several knowledge gaps concerning the exact mechanisms involved in the biosynthesis of bimetallic composites when used for the removal of arsenic species. Thus, this work focused on the biosynthesis mechanism involved in the formation of a Fe/Cu bimetallic bio-composite (Fe/Cu-OC), and determination of the specific biomolecules in tea extract involved in biosynthesis, and identification of the reactive sites involved in the removal of As(V). FTIR , XPS, GC-MS, and LC-MS analysis of the main components of the tea extract proved that the surface of Fe/Cu-OC contained many different functional groups, including -OH, Fe/Cu-O, and O C-OH, which were mainly associated with theanine and caffeine complexes. SEM and TEM analyses indicated that Fe/Cu-OC had both crystalline and amorphous features with an average particle size of 366 ± 10 nm. A 97 % removal efficiency for As(V) was obtained by Fe/Cu-OC, suggesting that the surface contained numerous reactive sites, including unsaturated Fe and Cu complexes, as well as saturated benzene rings. Moreover, DFT calculations indicated that the Gibbs free energy changes for the preparation of Fe/Cu-OC were < 0, suggesting that in the composites biosynthesis was a thermodynamically favored spontaneous reaction. A biosynthetic mechanism for the formation of Fe/Cu-OC was proposed, involving a series of spontaneous coordination, redox, and organic adsorption reactions.
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