CHEMICAL ENGINEERING JOURNAL
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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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MICROPOROUS AND MESOPOROUS MATERIALS
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2022
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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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SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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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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PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 47
·期 1
·192-202
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IF 3.925
Huanhuan Wang,Qi Qu,Zhiming Liu,Yan He,Jiangshan Gao
Herein, we report a micro-mix strategy for the continuous and large-scale synthesis of Ni–Co PBA nanoparticles. The technique presented in this study allows the particle size to be controlled in the 165 nm to 350 nm range while maintaining a high specific surface area (250 m2 g−1) and cubic structure. Furthermore, the particles exhibit superior dispersity and have a more homogeneous particle size than those prepared using the conventional stirring-mix method due to the drastic collisions that occur in the microchannel during the precipitation process. The present study demonstrates that the concentration of raw materials and feed flow rates in the microreactor effectively control the particle size during mixing. The high concentration of raw materials could decrease the particle size, and the particle size is decreased with the increasing feed flow rates when Re (Reynolds number) <783. Particularly, when 783 < Re < 1567, the particle size remains stable (about 165 ± 10 nm). Additionally, the space-time yield (STY) of Ni–Co PBA is 471 kg m−3 d−1. Finally, the continuous flow microreactor can continuously fabricate large-scale and high-quality Ni–Co PBA crystals with distinct morphological features in a short period of time, providing an effective alternative to the time-consuming and multi-step MOF synthesis method.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
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2023
·Vol. 24
·期 4
·3864
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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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ChemistrySelect
·
2022
·Vol. 7
·期 44
·e202203089
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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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Journal of Environmental Sciences
·
2022
·
IF 6.796
Jianhui Xu,Pengxu Wang,Shenggui Chen,Lei Li,Dan Li,Yunfei Zhang,Qi Wu,Jinhong Fan,Luming Ma
Here, we report the production of 3D-printed MoS 2 /Ni electrodes (3D-MoS 2 /Ni) with long-term stability and excellent performance by the selective laser melting (SLM) technique. As a cathode, the obtained 3D-MoS 2 /Ni could maintain a degradation rate above 94.0% for florfenicol (FLO) when repeatedly used 50 times in water. We also found that the removal rate of FLO by 3D-MoS 2 /Ni was about 12 times higher than that of 3D-printed pure Ni (3D-Ni), attributed to the improved accessibility of H*. In addition, the electrochemical characterization results showed that the electrochemically active surface area of the 3D-MoS 2 /Ni electrode is about 3-fold higher than that of the 3D-Ni electrode while the electrical resistance is 4 times lower. Based on tert -butanol suppression, electron paramagnetic resonance and triple quadrupole mass spectrometer experiments, a “dual path” mechanism and possible degradation pathway for the dechlorination of FLO by 3D-MoS 2 /Ni were proposed. Furthermore, we also investigated the impacts of the cathode potential and the initial pH of the solution on the degradation of FLO. Overall, this study reveals that the SLM 3D printing technique is a promising approach for the rapid fabrication of high-stability metal electrodes, which could have broad application in the control of water contaminants in the environmental field.
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ENGINEERING FAILURE ANALYSIS
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2022
·
IF 3.634
Anhua Ren,Min Kang,Xiuqing Fu
Ni/WC-MoS 2 composite coatings were fabricated in electrolytes with different MoS 2 doping levels using jet electrodeposition. We investigated the surface characteristics of Ni/WC-MoS 2 composite coatings, including the composition, surface morphology, microhardness and tribological behaviour. We also analysed the Ni/WC-MoS 2 composite coating wear mechanism during the wear process. The outcomes determined that Ni/WC-MoS 2 coatings had better surface quality, smaller grain size and larger coating thickness than Ni/WC coatings. The doping of MoS 2 promoted the deposition of WC in the coatings, which further enhanced the microhardness of the coatings. The Ni/WC-MoS 2 composite coatings doped at a MoS 2 concentration of 5 g/L exhibited a maximal microhardness of 730 HV 0.1 . Doping by MoS 2 effectively minimized the coefficients of friction ( CoFs ) of the composite coatings to 0.3. During the wear process, the repair effect of MoS 2 and formation of oxidised friction films transformed the adhesive wear into oxidative wear assisted by abrasive wear, which improved the abrasion resistance of the coatings and diminished the wear rate. The wear rate of the Ni/WC-5 g/L MoS 2 composite coating decreased by 47.34 % in comparison with that of coatings without MoS 2 doping, which was 7.44 × 10 4 μm 3 /N∙m. The findings indicate that doping MoS 2 can effectively enhance the surface wear resistance. This research provides a practical approach to prolong the service life of metal parts.
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FUEL
·
2022
·
IF 8.035
Zidan Zou,Chun Chen,Zhi Hu,Yue Shen,Zhen Fu,Wenchao Li,Yunxia Zhang,Haimin Zhang,Huijun Zhao,Guozhong Wang
Silica is one of the most referenced materials for the preparation of heterogeneous metal catalysts. However, silica spheres with smooth surfaces have difficulty encapsulating active metals due to their small surface area and the presence of only a handful of silicon hydroxyl groups on the surface. In this work, the silica sphere has been first consciously transformed into a hierarchical SiO 2 @silicate structure, and then the core–shell hetero-structured SiO 2 @Ni/SiO 2 catalyst can be tactfully obtained by reducing treatment. The core–shell catalyst is composed of a rigid core (SiO 2 ) and a rough shell (Ni NPs highly disperse on nanosheet SiO 2 ), which are carefully verified by X-ray diffraction (XRD), transmission electron microscope (TEM), field scanning electron microscope (FESEM), H 2 -TPR/TPD and X-ray photoelectron spectroscopy (XPS). The derived SiO 2 @Ni/SiO 2 catalyst can selectively hydrogenate vanillin in the aqueous phase at near-room temperature (40 ℃) and low hydrogen pressure (2 MPa H 2 ), and the conversion of vanillin can be up to 99%. The preparation method of the SiO 2 @Ni/SiO 2 catalyst is simple and can be amplified to a large scale at a low price, thus can be adopted to convert bio-derived unsaturated compounds in an economical and eco-friendly way.
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RENEWABLE ENERGY
·
2022
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IF 8.634
Feng Lin,Yulong Ma,Yonggang Sun,Zhi Song,Xiuqin Men,Yuhua Wu,Yingbo Zhu,Tingting Gao,Yudan Zhong
The catalytic upgrading of renewable lignin to value-added transportation fuels and chemicals is considered as the best solution to environmental and energy-related issues, however, such conversions are challenging. In this study, a new type of two-dimensional (2D) nanosheet catalyst, Ni/HZ5-NS (50 nm), was synthesized and used to catalyze the selective hydrodeoxygenation of a lignin model compound, 4-ethylguaiacol, to prepare renewable fuel precursors (C 8 –C 16 alkanes). The Ni/HZ5-NS catalyzed conversion of 4-ethylguaiacol to ethyl-cycloalkane reached 100%, and the product selectivity was greater than 95%. The microenvironment of the Ni species in Ni/HZ5-NS was regulated by HZ5-NS. The catalytic activity of Ni/HZ5-NS was twice than that of the traditional Ni/HZ5 catalyst. The high catalytic activity of Ni/HZ5-NS can be attributed to the synergy between the electron-rich Ni and the acidic sites on HZ5-NS but more importantly to the 2D nanosheet structure, which reduces the mass transfer resistance of the system and facilitates molecular diffusion. The application of Ni/HZ5-NS to catalyze C–O bond cleavage was extended to other lignin-derived aromatic ring compounds, and the conversion was found to reach 100%. Importantly cycloalkanes could be obtained with high selectivity. Therefore, this study will be useful for extracting alternative sources of valuable fuel precursors from biomass.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Shichao Zhang,Wenbin Chen,Junju Mu,Jianyu Han,Chaofeng Zhang,Zhuyan Gao,Jian Zhang,Yehong Wang,Feng Wang
Rapid kinetic adsorption and long-term cyclic stability are two of the major obstacles to the industrialization of solid amine adsorbents. The morphology and dispersibility of the organic amine in the pore structure of the support can strongly affect the adsorption rate and stability of CO 2 . In this work, we propose a strategy that enhances the dispersion and stability of tetraethylene pentamine (TEPA) via anchoring TEPA with single site Ni(II) in the pore of the commercial mesoporous silica gel (SG). The microscopic morphology and dynamic behavior of TEPA molecules in the adsorbents preparation process were explored by molecular dynamics simulation, which proved that the dispersibility of anchored TEPA in the porous structure has been improved, resulting in enhanced mass transfer and increased kinetic adsorption rate. The anchored Ni-TEPA/SG adsorbents exhibit a 37.5% faster kinetic adsorption rate than TEPA/SG adsorbents at 30 wt% TEPA loading, and the time required to reach 90% of maximum adsorption capacity is shortened by 6 times. Besides, the CO 2 adsorption performance of the optimized Ni-TEPA/SG adsorbent remains unchanged after 20 cycles, consolidating the potential of our proposed strategy in improving the kinetic adsorption rate and cyclic stability of solid amine adsorbents as well as promoting its industrialization.
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Green Energy & Environment
·
2022
·
IF 12.781
Ran Xi,Yiwei Tang,Richard Lee Smith,Xiaoning Liu,Le Liu,Xinhua Qi
Ni–Ru bimetallic porous carbon sphere (Ni–Ru@PCS) catalysts were synthesized via formaldehyde-assisted, metal-coordinated crosslinking sol–gel chemistry, in which biomass-derived tannic acid and F127 surfactant were used as carbon precursor and soft template, respectively, and Ni 2+ and Ru 3+ were used as cross-linkers. In the developed method, Ni–Ru particles became uniformly dispersed in the carbon skeleton due to strong coordination bonds between metal ions (Ni 2+ and Ru 3+ ) and tannic acid molecules and bimetal interactions. The as-synthesized Ni–Ru 10:1 @PCS catalyst with a loading Ni:Ru mole ratio of 10:1 was applied for the selective hydrogenation of glucose to sorbitol, and provided 99% glucose conversion with a sorbitol selectivity of 100% at 140 °C in 150 min reaction time and exhibited good stability and recyclability in which sorbitol yield remained at 98% after 4 cycles with little or no metal agglomeration. The catalyst was applied to glucose solutions as high as 20 wt% with 97% sorbitol yields being obtained at 140 °C in 20 h. The developed bimetallic porous carbon sphere catalysts take advantage of sustainably-derived materials in their structure and are applicable to related biomass conversion reactions.
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