JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Tingting Wei,Jie Bie,Wenqing Wei,Shuang Chen,Xiaobing Xu,Wei Fa,Xinglong Wu
The electrochemical oxygen evolution reaction is a bottleneck reaction in hydrolysis and electrolysis because the four-step electron transfer leads to slow reaction kinetics and large overpotentials. This situation can be improved by fast charge transfer by optimizing the interfacial electronic structure and enhancing polarization. Herein, a unique metal (Ni) organic (diphenylalanine, DPA) framework Ni(DPA) 2 (Ni-MOF) with tunable polarization is designed to bond with FeNi-LDH (layered double hydroxides) nanoflakes . The Ni-MOF@FeNi-LDH heterostructure delivers excellent oxygen evolution performance exemplified by an ultralow overpotential of 198 mV at 100 mA cm −2 compared to other (FeNi-LDH)-based catalysts. Experiments and theoretical calculations show that FeNi-LDH exists in an electron-rich state in Ni-MOF@FeNi-LDH due to polarization enhancement caused by interfacial bonding with Ni-MOF. This effectively changes the local electronic structure of the metal Fe/Ni active sites and optimizes adsorption of the oxygen-containing intermediates. Polarization and electron transfer of Ni-MOF are further enhanced by magnetoelectric coupling consequently giving rise to better electrocatalytic properties as a result of high-density electron transfer to active sites. These findings reveal a promising interface and polarization modulation strategy to improve electrocatalysis .
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Yuan-li Wang,Tong-hui Yang,Song Yue,Hang-bo Zheng,Xiao-pan Liu,Peng-zhao Gao,Hang Qin,Han-ning Xiao
Composition optimization, structural design, and introduction of external magnetic fields into the catalytic process can remarkably improve the oxygen evolution reaction (OER) performance of a catalyst. NiFe2O4@(Ni, Fe)S/P materials with a heterogeneous core–shell structure were prepared by the sulfide/phosphorus method based on spinel-structured NiFe2O4 nanomicrospheres. After the sulfide/phosphorus treatment, not only the intrinsic activity of the material and the active surface area were increased but also the charge transfer resistance was reduced due to the internal electric field. The overpotential of NiFe2O4@(Ni, Fe)P at 10 mA cm–2 (iR correction), Tafel slope, and charge transfer resistance were 261 mV, 42 mV dec–1, and 3.163 Ω, respectively. With an alternating magnetic field, the overpotential of NiFe2O4@(Ni, Fe)P at 10 mA cm–2 (without iR correction) declined by 45.5% from 323 mV (0 mT) to 176 mV (4.320 mT). Such enhancement of performance is primarily accounted for the enrichment of the reactive ion OH– on the electrode surface induced by the inductive electric potential derived from the Faraday induction effect of the AMF. This condition increased the electrode potential and thus the charge transfer rate on the one hand and weakened the diffusion of the active substance from the electrolyte to the electrode surface on the other hand. The OER process was dominantly controlled by the charge transfer process under low current conditions. A fast charge transfer rate boosted the OER performance of the catalyst. At high currents, diffusion exerted a significant effect on the OER process and low OH– diffusion rates would lead to a decrease in the OER performance of the catalyst.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 16
·7566-7574
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IF 3.3
Shengbiao Zheng,Tianna Liu,Nini Zhang,Liang Li,Yanli Zhu,Erhui Zhang,Jing Tang,Jiahao Guo
In this report, CoNi-bimetal metal–organic framework (CoNi-MOF) nanosheets with a three-dimensional (3D) flower-like hierarchical structure have been fabricated to modify a glassy carbon electrode and improve its efficiency for determination of quercetin. Scanning electron microscopy, X-ray photoelectron spectroscopy, N2 adsorption–desorption isotherms and impedance spectroscopy were used for the characterization of the CoNi-MOF. Under optimal electrochemical conditions, the anodic peak current measured around 0.44 V (vs. SCE) increased linearly in two linear ranges: 0.05 to 1.0 μM and 1.0–20 μM with a sensitivity of 13.21 μA μM−1 cm2 and 0.934 μA μM−1 cm2, respectively. The excellent electrochemical performance might be attributed to the hierarchical structure, large specific surface area and enhanced electrical conductivity. Finally, the analytical utility of the CoNi-MOF sensor was evaluated by detecting quercetin in human plasma samples.
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Analytical Methods
·
2023
·Vol. 15
·期 14
·1819-1825
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IF 3.1
Jing Wan,Jian-Mei Zou,Shu-Jing Zhou,Feng-Lan Pan,Fei Hua,Yu-Lan Zhang,Jin-Fang Nie,Yun Zhang
A novel nanozyme of bimetallic (Ni/Co) metal–organic framework (Ni/Co-MOF) was synthesized using a simultaneous precipitation and acid etching method with a zeolitic imidazolate framework ZIF-67 as the template. The as-synthesized Ni/Co-MOF catalyst presented a three-dimensional hollow nanocage structure and exhibited excellent intrinsic oxidase-like activity. It was demonstrated that Ni/Co-MOF could directly catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to produce a blue product (oxidized TMB, oxTMB) in the absence of H2O2. The mechanisms and kinetics of this nanozyme activity were investigated, and it was determined that the catalytic activity of Ni/Co-MOF was closely related to temperature and solution pH. Owing to its strong reducibility, ascorbic acid (AA) could reduce oxTMB, and the blue color of the reaction mixture faded over time. Therefore, a novel colorimetric platform was constructed to detect AA based on the oxidase-like activity of Ni/Co-MOF. Under optimal conditions, the absorbance of ox-TMB at 652 nm decreased linearly over the 0.015–50 μM AA range with a detection limit of 0.004 μM.
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Biomass Conversion and Biorefinery
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2023
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IF 4
Nie Fahui,Guan Kun,Zou Chenglong,Xu Zhiwei,Liu Zhanmeng
Ferrate, as an internal oxidation modifier, is rarely used in the preparation of magnetic biochar. This research promotes rice shell charcoal modified by K 2 FeO 4 preparation of oxygen-containing groups and ɤ-Fe 2 O 3 magnetic biochar. Magnetic rice husk biochar (MBC) is prepared to adsorb Ni(II) from aqueous solutions. The effects of various parameters on the adsorption of Ni(II) by MBC have been studied, and the results show that MBC has an excellent adsorption capacity for Ni(II). At 25 °C and pH 7.0, the removal rate of Ni(II) reaches 96.1% within 24 h at an adsorbent dose of 0.5 g/L when the initial Ni(II) concentration is 20 mg/L. The kinetic model conforms to the pseudo-second-order kinetic model and the intra-particle diffusion model within 36 h. Moreover, the adsorption data were successfully reproduced by the Langmuir isotherm, and the maximum adsorption capacity is 42.69 mg/g. The adsorption data conform to the D-R model, and the calculated average adsorption free energy is 41.03 kJ/mol, indicating that the adsorption process is mainly chemical adsorption. Thermodynamic study indicates that the endothermic adsorption process is spontaneous and can be promoted by the increase in temperature. This study was expected to provide a reference and theoretical basis for the treatment of Ni(II)-containing wastewater using modified rice husk biochar.
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RENEWABLE ENERGY
·
2023
·
IF 8.7
Mengxue Song,Chonghao Qiu,Pengfei Ma,Jiawei Zhong,Zhuohan Zhang,Weiping Fang,Wenjing Song,Jianqiang Fan,Weikun Lai
Reductive etherification is an attractive and practical strategy to convert bio-platform compounds into valuable chemicals. In directed synthesis of furfuryl ethers, reductive etherification of bioderived furfurals is still challenging due to the complexity of catalytic reaction . Herein, reductive etherification of furfural with alcohol was investigated over Ni/ZSM-5 catalyst, which found that Si/Al ratios in ZSM-5 played an important role on the catalytic performance. For Ni/ZSM-5 with Si/Al ratio of 50, 80.9% yield of furfuryl ether at 90.8% conversion of furfural was achieved under the condition of 2 MPa H 2 and 180 °C for 3 h in isopropanol. The catalyst exhibited superior stability and recyclability during the consecutive cycle run. Catalysts characterization demonstrated that both acidic properties and furfural adsorption were influenced by the Si/Al ratios in Ni/ZSM-5, which correlated to the reaction route and catalytic performance. Lewis acid sites enhanced furfural hydrogenation into furfuryl alcohol, while Brønsted acid sites on ZSM-5 effectively catalyzed sequential etherification of furfuryl alcohol to furfuryl ether. Under optimization conditions, various furfuryl ethers could be obtained with yields above 80% over Ni/ZSM-5 catalyst in different primary alcohols, demonstrating the general versatility of the approach. Our findings offered opportunities to develop an efficient furfuryl ethers synthesis method .
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Jianping Ai,Yaping Shuai,Min Hu,Lihong Cheng,Siling Luo,Wenkui Li,Zhiqin Chen,Liling Hu,Zehua Zhou
A novel class of high-entropy (HE) spinel ferrites (Mg 0.2 Co 0.2 Ni 0.2 Cu 0.2 Zn 0.2 )Fe 2 O 4 , have been successfully synthesized by the solution combustion synthesis method followed by heat-treatment at 500–1500 °C. The resultant spinel ferrites were systematically investigated by various methods including XRD , SEM, TEM, EDS, Raman spectra, etc. It was demonstrated that the entropy drives a reversible transformation between a single-phase state and multiphase. And the entropy predominates the thermodynamic landscape. The as-fabricated high-entropy (Mg 0.2 Co 0.2 Ni 0.2 Cu 0.2 Zn 0.2 )Fe 2 O 4 solid solution is single-phase with homogeneous transition-metal element distribution. Moreover, a trade-off between grain growth and crystallization during heat-treatment process; the average grain size of product is only 352.96 nm after being annealed at 1000 °C for 3 h probably due to “sluggish diffusion effect”. The resultant HE spinel ferrites (Mg 0.2 Co 0.2 Ni 0.2 Cu 0.2 Zn 0.2 )Fe 2 O 4 were first used as a heterogeneous catalyst of peroxodisulfate (PDS). Compared with basic solution condition, the HE spinel ferrite/PDS system exhibited a higher degradation rate for the removal of rhodamine B (RhB) and tetracycline (TC) at initial pH range of 3.0–5.1. Both the hydroxyl radicals and sulfate radicals played an important role on RhB and TC degradation. The high catalytic efficiency and good stability of high-entropy (Mg 0.2 Co 0.2 Ni 0.2 Cu 0.2 Zn 0.2 )Fe 2 O 4 catalyst demonstrates that it is suitable for application in wastewater disposal.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2023
·Vol. 24
·期 4
·3864
·
IF 5.6
Kangjing Wang,Liting Zhao,Ting Li,Qian Wang,Zhongyang Ding,Weifu Dong
Ion exchange resins are suitable as carriers for immobilized enzymes because of their stable physicochemical properties, appropriate particle size and pore structure, and lower loss in continuous operation. In this paper, we report the application of the Ni-chelated ion exchange resin in the immobilization of His-tagged enzyme and protein purification. Acrylic weak acid cation exchange resin (D113H) was selected from four cationic macroporous resins that could chelate the transition metal ion Ni. The maximum adsorption capacity of Ni was ~198 mg/g. Phosphomannose isomerase (PMI) can be successfully immobilized on Ni-chelated D113H from crude enzyme solution through chelation of transition metal ions with the His-tag on the enzyme. The maximum amount of immobilized PMI on the resin was ~143 mg/g. Notably, the immobilized enzyme showed excellent reusability and maintained 92% of its initial activity with 10 cycles of catalytic reaction. In addition, PMI was successfully purified using an affinity chromatography column prepared by Ni-chelated D113H, which showed the potential for the immobilization and purification process to be realized in one step.Keywords:ion exchange resin;His-tag;immobilization;enzyme activity;protein purification;reusability
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Guangyu Duan,Xintong Li,Xin Ma,Wei Zhong,Shuai Wang
Cu/Ni-bearing wastewater contamination has recently been a challenge for the environmental protection worldwide. Herein, a novel poly(2-acrylamide-pentanedihydroxamic acid) (PAPDA) resin containing –CONHOH and –COOH groups was prepared and applied to effectively remove Cu 2+ and Ni 2+ from heavy metal wastewater. The batch adsorption experiments revealed that the maximum adsorption capacities of PAPDA resin for Cu 2+ and Ni 2+ were 436.08 and 195.05 mg·g −1 , respectively, which were 10.20 and 9.45 times higher than that of polyacrylic resin . Specifically, the adsorption kinetics and thermodynamics of PAPDA were respectively consistent with the pseudo-second-order kinetic model and the Langmuir isotherm model, indicating that the adsorption is a single-layer chemisorption process. Besides, the adsorption mechanism was investigated by SEM, XRD, FT-IR, XPS, DFT calculations, suggesting that the PAPDA resin possessing abundant active sites could effectively adsorb the heavy metal ions . Noticeably, the –CONHOH groups represented the strong affinity towards Cu 2+ and Ni 2+ by forming stable five-membered rings. In addition, column experiments were conducted to study the practical adsorption process of PAPDA resin to heavy metal ions. Overall, the results proved that the novel PAPDA resin as a green and highly efficient adsorbent has a promising potential for the treatment of heavy metals-containing wastewater.
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ChemistrySelect
·
2022
·Vol. 7
·期 44
·e202203089
·
IF 2.307
Lei He,Tuanhui Li,Xiaoxuan Zhang,Shizhong Luo,Zhisheng Shi,Ruirui Yun
Graphical An embedded Ni-based catalysts have been designed and synthesized by a biopolymer-assistant strategy which followed by calcination under different temperature. Among of them, Ni@PC-900 shows an excellent activity and chemo-selectivity for the hydrogenation of nitroarenes under mild conditions, even in the present of alternative unsaturated groups. Considering of the fact that many of the catalysts reported previously show low selectivity in the hydrogenation reaction. Herein, a series of nickel particles embedded in porous carbon have been synthesized by bio-template strategy. Among of them, Ni@PC-900 (PC: porous carbon; 900: the pyrolysis temperature) shows higher activity and selectivity (conversion>99 % within 30 minutes under room temperature) than that of other catalysts. All of the characterizations of the as-synthesized indicate that the high catalytic activity has a positive correlation with the particle size and distribution of the particles. Moreover, Ni@PC-900 also exhibits excellent durability maybe due to the well core-shell structure protecting the active site from leaching during the catalytic process.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Runjie Li,Yanyan Zhang,Bing Xing,Mengtian Huang,Ting Wang,Xiaoping Hong,Baocheng Zhou,Benxia Li,Jia Ding,Qi Sui
The selective oxidation of alcohols by transition-metal-based catalysts provides a green route for the production of aldehydes. In this paper, mesoporous SBA-15 supported bimetallic Ni x Co y oxides were synthesized for the catalytic oxidation of alcohol using oxygen as the sole oxidant. The catalytic activity was highly related to the metal composition, of which the Ni 1 Co 4 /SBA-15 catalyst showed the best catalytic performance with high benzyl alcohol conversion of 96.2% and benzaldehyde selectivity of 98.3%. It was proposed that the electronic structure of the Ni x Co y /SBA-15 catalysts can be modulated by Ni/Co ratio, and high Co 3+ /Co 2+ and Ni 3+ /Ni 2+ ratios promoted the catalyst activity. Compared to the Ni x Co y nanocatalysts obtained by removing SBA-15 support, the Ni x Co y /SBA-15 exhibited a better benzyl alcohol oxidation performance, suggesting a diffusion enhancement by the mesoporous structure of SBA-15 support.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Bin Han,Yuanfang Lin,Yu Luo,Weizhen Liu,Xueming Liu,Zonglin Weng,Xinwen Ou,Zhang Lin
Low-crystalline ultrathin nanosheets (UNSs) hold great potential for efficient photoreduction of anthropogenic CO 2 , while developing green synthetic methodologies and elucidating the structure-performance relationship remain significant challenges. Here, via a CaO-mediated strategy , we demonstrate a facile strategy for the large-scale production of low-crystalline Ni(OH) 2 UNSs from industrial wastes. The resultant Ni(OH) 2 UNSs deliver a superior CO formation rate of 9.2 μmol h −1 with a high selectivity of 93.1 % in low-concentration CO 2 (10 %), which remarkably outperforms that of Ni(OH) 2 NSs with high crystalline. Experimental and theoretical investigations demonstrate that the boosted performance originates from the fully exposed oxygen vacancies and low-coordination Ni sites, which facilitates the separation of photogenerated charge pairs and the adsorption and activation of diluted CO 2 . This work demonstrates a sustainable strategy for the large-scale synthesis of low-crystalline layered metal hydroxides, paving new avenues for the high-value utilization of industrial wastes in mitigating climate change.
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