CHEMBIOCHEM
·
2021
·Vol. 23
·期 4
·e202100497
·
IF 3.164
Kangjing Wang,Liting Zhao,Ting Li,Qian Wang,Zhongyang Ding,Weifu Dong
Graphical Phosphomannose isomerase (PMI) with His-tag was successfully immobilized on Ni 2+ charged pyridine-derived particles. The immobilized enzymes effectively maintained their activity. Excellent reusability and stability was observed after immobilization. Self-stable precipitation polymerization was used to prepare an enzyme-immobilized microsphere composite. Phosphomannose isomerase (PMI) with His-tag was successfully immobilized on Ni 2+ charged pyridine-derived particles. The maximum amount of PMI immobilized on such particles was ∼184 mg/g. Compared with free enzyme, the activity of the immobilized enzymes was significantly improved. In addition, the immobilized enzymes showed a much better thermostability than free enzymes. At the same time, the immobilized enzymes can be reused for multiple reaction cycles. We observed that the enzyme activity did not decrease significantly after six cycles. We conclude that the pyridine-derived particles can be used to selectively immobilize His-tagged enzymes, which can couple the enzyme purification and catalysis steps and improve the efficiency of enzyme-catalyzed industrial processes.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 51
·2306868
·
IF 19
Zhipeng Jiang,Tao Yang,Chen Li,Jiahang Zou,Hanxu Yang,Qingan Zhang,Yongtao Li
Ether-based electrolytes have high ionic conductivity and good stability toward the lithium metal anode relative to carbonate-based electrolytes, but they typically exhibit poor oxidation stability (<4 V vs Li + /Li). Most approaches aimed at enhancing the oxidative stability of ether-based electrolytes, such as “salt-in-solvent” and “weakly solvating” strategies, often sacrifice their inherent advantage of high ionic conductivity. Herein, this article proposes a cost-effective synergistic additive strategy by co-adding LiNO 3 and vinylene carbonate (VC) to achieve an optimized ether-based electrolyte (OEE) that simultaneously offers high Li-ion (Li + ) conductivity (11.52 mS cm −1 at 20 °C) and high-voltage stability (4.4 V). LiNO 3 and VC can enter the inner solvation shell of the electrolyte, preferentially participating in the film-forming progress at the electrode surface, leading to the formation of a unique organic–inorganic bilayer interfacial protective layer. This layer could effectively suppress electrolyte side reactions and enhance electrode stability. As a result, the 4.4 V Li-LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NCM811) full cells assembled with the OEE exhibit stable cycling performance at both room temperature and low temperature. This work provides a new approach to the design of ether-based electrolytes for high-voltage lithium metal batteries.
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ENERGY & FUELS
·
2023
·
IF 5.3
Yi Ren,Yujia Bai,Genxiang Wang,Yijian Liu,Chuancheng Mou,Jiayu Chen,Baohuan Wei,Hui Wang,Yuhan Sun
Efficient conversion of CO2 to value-added fuels or chemicals using electricity from renewable sources is an appealing approach to realize carbon neutrality. Under this background, it is crucial to design efficient and low-cost catalysts for CO2 electroreduction. Herein, we fabricated an electrocatalyst with the structure of Cu–Ni alloy nanoparticles grown on nitrogen-doped carbon nanotubes (CuxNi/NCNT, x = 2.4, 1, and 0.36) for electrochemical CO2 reduction reaction (CO2RR) via a hydrothermal method followed by pyrolysis. The optimized CuNi/NCNT demonstrates a favorable CO2RR performance with a CO Faradaic efficiency (FECO) of 94.8% and a current density of 26.6 mA cm–2 at −0.9 V versus the reversible hydrogen electrode (vs RHE) in the H-cell, far superior to those of single metal counterparts. Density functional theory (DFT) calculations unravel that the Cu–Ni alloys possess much lower free energy changes for the formation of the key COOH* intermediate than those of the Cu metal, thereby facilitating CO2 reduction into CO. Additionally, the CO2RR performance of CuNi/NCNT was further evaluated in the gas diffusion electrode (GDE) involved in the flow cell to examine the practical application of the prepared catalyst, which can deliver a current density of 124.6 mA cm–2 with a FECO of 92.8% at −1.1 V vs RHE. This work enriches electrocatalysts for highly efficient CO2 electroreduction to CO.
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CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
·
2023
·
IF 2.2
Hongye Bai,Lihao Yu,Jinfu Xu,Xuliang Pang,Yajie Bai,Jianguo Cui,Weiqiang Fan
Decoration of metal-organic framework (MOF) has been considered as an effective route to improve the photoelectrochemical (PEC) performance of TiO 2 , but there is still a lack of understanding of the regulatory structure. Herein, Ni-MOF was rationally introduced by in-situ etching method, which helps for artificially regulating the coordination state of Ni sites. The photocurrent density (0.81 mA/cm 2 ) and IPCE value (33.1%) of TiO 2 -MOF-2 are about twice higher than that of pristine TiO 2 due to the rich unsaturated sites of Ni-MOF. Meanwhile, the saturated coordination has caused the decline of PEC performance because of the obvious steric hindrance . Therefore, this work presents an insight for the effect of coordination state on PEC activity especially in MOF system.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Xuan Liu,Jianying Wang,Zhongying Fang,Shuaiqi Gong,Dengke Xiong,Wei Chen,Deli Wu,Zuofeng Chen
Herein, an ultrafast electro-corrosion approach is developed for activating Ni foam (NF) into an efficient electrocatalyst for upcycling polybutylene terephthalate (PBT) waste plastic. The electro-corrosion process assisted by Cl − is completed by only 6 CV cycles (∼3 min) and the activity of the treated NF (T-NF), characterized by the integrated Ni 2+ /Ni 3+ peak area is enhanced by 150 times. The T-NF electrode exhibits excellent catalytic activity toward 1,4-butanediol oxidation , delivering a current density of 50 mA cm − 2 at 1.36 V (vs. RHE). This allows the electrocatalytic reforming of 1,4-butanediol component in PBT hydrolysate into succinate with a high Faraday efficiency 93%. The in-situ Raman and FTIR spectroscopies combining density functional theory calculations identify catalytically active centers, critical intermediates, and favorable pathway for 1,4-butanediol oxidation to succinate. This work provides an ultrafast one-step surface engineering strategy to turn pristine Ni foams into high-performance electrocatalysts for upcycling PBT plastic and other electrochemical applications.
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ACS Catalysis
·
2023
·
IF 12.9
Dong Ji,Peng Guo,Yongjie Xi,Jinlei Li,Jia Wang,Tingting Wang,Fuwei Li
Selective tandem hydrogenation is a promising strategy for catalytic conversion of bulk raw materials with multifunctional groups into high-value-added chemicals via multiple-step reactions. Yet now, one of the current challenges is to develop a multifunctional and stable catalyst enabling the tandem catalysis rather than interrupting at any step reaction, particularly for supported nonprecious metal catalysts. In this work, we report tandem hydrogenation of bulk phthalic anhydride toward the one-pot synthesis of hexahydrophthalide, an emerging monomer of a recyclable polyester, over phosphorus-promoted Ni–Co bimetallic alloy nanoparticle catalysts. The surface composition of catalysts can be easily regulated by changing the Ni/Co molar ratio and the phosphorous functionalization strategy, which could then tune the product selectivity and enhance the stability of this tandem process. The optimal Ni3Co1@NC-P affords 88% selectivity for the desired product and demonstrates promising stability toward the tandem hydrogenation reaction. Systematic experimental and computational studies reveal that the adsorption strength of the intermediates and the ability of hydrogen activation can be altered by the formation of surface metallic Ni species, thus tuning the product selectivity. In addition, the oxidation resistance of Ni3Co1@NC-P was enhanced by the phosphorization treatment, which makes the bimetallic alloy successfully realize the tandem hydrogenation reaction. The finding of this work not only provides a convenient strategy to design and develop efficient and stable non-noble metal-based catalysts for selective tandem hydrogenation reactions, especially involving the hydrodeoxygenation reaction, but also fulfills the straightforward pathway for the preparation of degradable polyester monomer hexahydrophthalide.
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Nanoscale
·
2023
·Vol. 15
·期 18
·8255-8269
·
IF 6.7
Huanhuan Wang,Qi Qu,Jiangshan Gao,Yan He
Herein, Fe3O4@MnO2@Ni–Co/C composites derived from PBAs were successfully fabricated. Firstly, Ni–Co Prussian blue analogues (Ni–Co PBAs) were used as precursors to derive a carbon layer on their surface by annealing treatment and subsequently translated into MnO2@Ni–Co/C nanocubes after hydrothermal reactions. Fe3O4@MnO2@Ni–Co/C composites were finally obtained after depositing Fe3O4 nanoparticles through the annealing process. Their electromagnetic wave (EMW) absorption performance apparently enhanced, thanks to the excellent impedance matching and strong attenuation derived from the synergy between the dielectric loss and the magnetic loss. In particular, the minimum reflection loss (RLmin) of Fe3O4@MnO2@Ni–Co/C reached −41.2 dB with a thickness of 4.0 mm and the effective absorption bandwidth (EAB) reached 7.1 GHz with a thickness of 2.0 mm. Therefore, the results could be significant for synthesizing EMW absorbers with excellent performance, a broad bandwidth, strong absorption, thin thickness and light weight.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Xianglei Cao,Liugen Zhang,Changyan Guo,Tingxiang Chen,Chao Feng,Zechang Liu,Ying Qi,Wei Wang,Jide Wang
In this paper, Ni x Cd y S composite photocatalysts were synthesized by using Ni-doped Cd–Co PBA as the precursor, which retains the advantages of PBA such as porous structure , large specific surface and highly dispersed metal active sites. The photocatalytic hydrogen production performance over Ni x Cd y S is three times higher than that of pure CdS with H 2 yield of 8.45 mmol g −1 h −1 . The catalyst was analyzed by the UV/Vis absorption spectra , photoluminescence spectra, time-resolved photoluminescence spectra, transient photocurrent responses, electrochemical impedance spectra, Mott-Schottky test, etc. A series of characterization results prove that the electron-hole recombination rate, electrochemical resistance and band gap of nickel-doped CdS composites are obviously smaller than CdS, which are important factors to improve the photocatalytic hydrogen production performance. This work may provide some reference value for the fabrication of other functional materials using PBA as precursors.
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ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Jiang Liao,Ao Ju,Wenhao Jiang,Yan Ju,Xueliang Liu,Nianxiang Hu,Ruidong Xu,Junli Wang
Transition metal hydroxides, due to their low cost and high theoretical capacity, are promising candidates for supercapacitors . However, the lower conductivity of hydroxides usually results in devices exhibiting poor specific capacity. Here, Ni(OH) 2 @Ni 12 P 5 electrodes are designed and prepared, showing great potential for applications. This composite electrode, prepared by simple phosphating treatment and electrodeposition . Compared with the Ni(OH) 2 prepared by direct deposition, this rationally designed electrode exhibits more excellent electrochemical properties. The prepared Ni(OH) 2 @Ni 12 P 5 electrode exhibits a good area specific capacitance of 15.89 F•cm −2 at a current density of 10 mA•cm −2 , which is 2.93 times higher than that of the Ni(OH) 2 electrode (5.43 F•cm −2 ). In addition, the assembled Ni(OH) 2 @Ni 12 P 5 //AC asymmetric supercapacitor exhibits an energy density of 0.38 mWh•cm −2 at a power density of 8.00 mW•cm −2 . Therefore, this work provides a new strategy for the synthesis of high-performance supercapacitor electrodes.
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Journal of Materials Chemistry A
·
2021
·Vol. 10
·期 11
·6007-6015
·
IF 12.732
Min Li,Minmin Wang,Dongyuan Liu,Yuan Pan,Shoujie Liu,Kaian Sun,Yanju Chen,Houyu Zhu,Wenyue Guo,Yanpeng Li,Zhiming Cui,Bin Liu,Yunqi Liu,Chenguang Liu
Single-atom catalysts (SACs) regulated by heteroatoms have displayed great potential as electrocatalysts for highly efficient hydrogen evolution reaction (HER); however, the controllable synthesis of an axial coordination structure of SACs to achieve robust HER performance remains a great challenge. Herein, we have proposed a doping-adsorption-pyrolysis strategy to construct NiN4–Cl active sites with axial Cl coordination for accelerating electrocatalytic HER. The obtained NiN4–Cl SAs/NC catalyst exhibits superior HER activity with low over-potential, small Tafel slope, high turnover frequency, and long-term stability. Density functional theory calculation reveals that the excellent HER performance of NiN4–Cl SAs/NC originates from the axial Cl-coordination-induced electronic localization enhancement, which is beneficial for the adsorption and activation of H* intermediate, thus accelerating the HER process. This work opens a new opportunity for rational design and construction of high-performance SAC catalysts by axial coordination strategy for electrocatalytic application.
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Mengting Zhu,Jiamin Shi,Xing Xin,Jinghua Wu,Xiayin Yao
All-solid-state lithium (Li) batteries have been emerging as attractive technologies for energy storage systems due to their benefits in safety. However, the electrochemical performance of all-solid-state Li batteries is limited by the interfacial problems resulting from the solid–solid contact between electrolytes and electrodes. Here, a binary transition-metal sulfide NixCo3–xS4 with a special hexagonal layered structure is synthesized and introduced into all-solid-state Li batteries based on sulfide electrolytes. By freely adjusting the Ni/Co ratio, components with optimal performance can be easily obtained. In addition, the well-designed interfacial structure is favorable for ion transport and interfacial stability because the sulfide electrolyte particles can rivet on the hexagonal platelets which can maximally reduce the contact resistance between the solid electrolytes and cathodes. As a result, the all-solid-state Li battery employing the Ni0.3Co2.7S4@Li7P3S11 composite cathode exhibits enhanced rate capability and cycling stability. At a current density of 0.1 A g–1, it delivers a specific capacity as high as 1216 mA h g–1. Even under a large current of 1 A g–1, a large capacity of 510 mA h g–1 can be retained after 100 cycles.
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Scientific Reports
·
2021
·Vol. 11
·期 1
·1-11
·
IF 4.38
Wang Haitao,Zou Haiyan,Liu Yingying,Liu Zhenglong,Sun Wenshuang,Lin Kunyi Andrew,Li Tielong,Luo Shuangjiang
It’s highly desired but challenging to synthesize self-supporting nanohybrid made of conductive nanoparticles with metal organic framework (MOF) materials for the application in the electrochemical field. In this work, we report the preparation of Ni 2 P embedded Ni-MOF nanosheets supported on nickel foam through partial phosphidation (Ni 2 P@Ni-MOF/NF). The self-supporting Ni 2 P@Ni-MOF/NF was directly tested as electrode for urea electrolysis. When served as anode for urea oxidation reaction (UOR), it only demands 1.41 V (vs RHE) to deliver a current of 100 mA cm −2 . And the overpotential of Ni 2 P@Ni-MOF/NF to reach 10 mA cm −2 for hydrogen evolution reaction HER was only 66 mV, remarkably lower than Ni 2 P/NF (133 mV). The exceptional electrochemical performance was attributed to the unique structure of Ni 2 P@Ni-MOF and the well exposed surface of Ni 2 P. Furthermore, the Ni 2 P@Ni-MOF/NF demonstrated outstanding longevity for both HER and UOR. The electrolyzer constructed with Ni 2 P@Ni-MOF/NF as bifunctional electrode can attain a current density of 100 mA cm −2 at a cell voltage as low as 1.65 V. Our work provides new insights for prepare MOF based nanohydrid for electrochemical application.
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