Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Yueling Yu,Jia Yang,Baogang Zhao,Xinfei Fan,Yuanlu Xu,Yanming Liu
Nonradical-based peroxymonosulfate (PMS) activation has recently caught increasing attention due to its less susceptible to environmental interference in the complex water matrix, but the performance of activators still requires further development for efficient pollutants degradation in wastewater treatment . Herein, a novel Co-Ni bimetal oxide loaded biochar was fabricated to boost nonradical PMS activation for enhancing sulfamethoxazole (SMX) degradation. According to the results, the as-obtained catalyst exhibited excellent SMX degradation efficiency of 96.2% within 30 min through complete nonradical oxidation pathway (including both 1 O 2 and mediated electron transfer). Co was confirmed to be the active sites to generate 1 O 2 dominated nonradical pathway. The biochar acted as the porous material to achieve the electron transfer oxidation process, as well as Ni ensured sufficient electron transfer rate and bound Co active sites to prevent the leaching of metal ions . Meanwhile, the prepared Co-Ni bimetal oxide loaded biochar possessed a remarkable catalytic degradation durability in the complex water environment conditions and showed universality for various organic contaminants . This study offers a valuable clue on the rational design of novel catalyst to induce the nonradical pathway-based persulfate activation .
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Journal of Materials Research and Technology-JMR&T
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2023
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IF 6.4
Zhenzhen Feng,Xiaomeng She,Jian Peng,Yujie Qiang,Song Zhang
Although magnesium alloys have been effectively used in industry, they have weak corrosion resistance. Herein, robust Ni-thiolate coordination polymer Mg(OH) 2 coatings were prepared by an oxidation-hydrolysis-coordination (OHC) strategy to make AZ31 magnesium alloy highly resistant to corrosion in 3.5 wt% NaCl solution. The OHC process includes three steps: I) oxidation of AZ31 to produce AZ31@MgO; II) hydrolysis of MgO to produce Mg(OH) 2 , cation exchange between Mg(OH) 2 and Ni(II) to produce Mg–Ni LDH; III) coordination of Ni(OH) 2 from Mg–Ni LDH by the 1,4-Benzenedithiol (BDT) ligand to produce LDH-BDT coatings. Potentiodynamic polarization, EIS, and in situ SRET in 3.5 wt% NaCl solution were used to assess the hybrid coating's anti-corrosion performance. Surprisingly, LDH-BDT coating achieves excellent corrosion inhibition performance (99.9999%) with the i corr of 1.926 × 10 −10 A cm −2 , which is six orders of magnitude lower than that of AZ31 substrate, this is due to the cooperative effect, such as the physical protection provided by thick LDH-BDT coatings and the hydrophobic properties of Ni(II)-BDT coordination polymers. This study provides fresh insight into the fabrication of Mg(OH) 2 -based coatings modified with Ni-thiolate complex to significantly improve Mg alloys' resistance to corrosion.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 51
·2306868
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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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Molecular Catalysis
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2023
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IF 4.6
Shide Wu,Yifei Zhang,Feng Yi,Dan Ping,Wan Li,Siyuan Cheng,Duwei Fan,Lifeng Han,Shiwen Wang,Junfeng Tian,Shaoming Fang
Developing an efficient and low-cost bifunctional electrocatalysts with superior activity for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is highly required but still challenging. Herein, highly dispersed Ni species containing both Ni nanoparticles (NPs) and atomically dispersed Ni-N X on mesoporous nitrogen-doped carbon (Ni-N-C) were prepared by a facile one-pot pyrolysis strategy using dicyandiamide, citric acid and nickel acetylacetonate as raw materials. The confinement agent citric acid is quite requisite for dispersing Ni NPs and forming mesoporous graphene-like carbon substrate. Due to the uniform size of Ni NPs (3 nm) and the synergistic effect between Ni NPs and Ni-N X , and the unique mesoporous carbon structure, such Ni-N-C catalyst exhibits favorable activities for both HER and OER. The overpotentials for HER and OER are only 218 and 330 mV vs. RHE on glassy carbon to deliver a current density of 10 mA·cm −2 , respectively. Moreover, this catalyst also showed good operation durability with no obvious deactivation after long-term (18 h) potentiostatic electrolysis or continuous CV tests. This work could offer a new avenue for the design of bifunctional electrocatalysts in efficient water splitting.
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APPLIED ENERGY
·
2023
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IF 11.2
Xiangyu Yan,Buchu Lu,Hao Dong,Qibin Liu
Combining solar light and heat in dry reforming of methane (DRM) is a promising technology for reducing CO 2 to a valuable syngas and increasing the utilization of solar light in the solar-to-fuel process. The reaction temperature is still high and the mechanism remains unclear in DRM. Clarifying the synergistic mechanism of solar light and heat is pivotal for industrial applications. To this end, a nanoscale Ni/CeO 2 catalyst is prepared, and the synergistic effect of solar light and heat in DRM is experimentally investigated. The experimental results show that photo-thermochemistry leads to a 39.74% increase in relative conversion rate of CH 4 compared to thermochemistry, while the reaction temperature is reduced by 45 °C. The syngas production rate and the selectivity of DRM are improved by solar light. The in-situ infrared study indicates that solar light enhances the dissociation process of CH 4 and the production of HCOO ⁎ on the surface of the Ni/CeO 2 catalyst. The light response in the catalyst and microscopic enhancement of intermediate products are responsible for the increased DRM performance under photo-thermochemical conditions. These findings contribute to the understanding of the synergistic effects of solar light and heat, and guide the conversion of CO 2 into fuel with the aid of solar energy.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yuxin Liu,Yiqiang He,Chunguang Li,Zhan Shi,Shouhua Feng
Photocatalytic technology is considered a sound solution to exploit hydrogen energy. Currently, photocatalytic hydrogen production and organic synthesis under simulated sunlight simultaneously have enormous practical significance. Herein, we synthesized Ni@C metal nanoparticles cocatalyst to form a composite photocatalyst with Indium-vacancy-rich In 2 S 3 by the electrostatic self-assembly method. The composite exhibited a hydrogen production rate of 3.52 mmol·g −1 ·h −1 and coupling of benzylamine 8.37 mmol·g −1 ·h −1 . X-ray photoelectron spectroscopy and density functional theory explored the reaction process and mechanism. The charge density difference of the heterojunction surface revealed that the Ni@C interacted with the substrate via both electrostatic interaction and chemical bonds. This confirmed that the electrons rapidly transferred to the cocatalyst under the irradiation of visible light, which was conducive to the surface reduction reaction and greatly inhibited the photogenerated carrier recombination. Moreover, hydrogen adsorption energy further explained the synergistic effect of co-modification of the defect and the fact that noble-metal-free cocatalyst could improve photocatalytic efficiency. This work offers insights into the preparation of new types of photocatalysts which produce hydrogen and high-value chemicals in the future.
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FUEL
·
2023
·
IF 7.4
Wenqi Zhao,Xiaowei Bai,Xiangrui Lin,Yalkunjan Tur sun,Mei Zhong,Zhenghua Dai,Jian Li
Biomass-derived furfural and its derivatives are promising feedstocks for producing valuable C 5 diols by catalytic hydrolysis. However, this process requires selective ring opening of tetrahydrofurfuryl alcohol (THFA) to 1,5-pentanediol, which is challenging. Here we report efficient route for this conversion using Ni-La(OH) 3 catalysts prepared by a green co-precipitation-hydrothermal method. We show that these catalysts can achieve up to 91.7% yield and 94.6% selectivity of 1,5-pentanediol from THFA under mild conditions. We elucidate the key role of the La(OH) 3 phase, the basic sites and the Ni n+ -O-La 3+ structure of the catalysts in promoting the selective hydrogenolysis and ring opening of THFA. We also demonstrate that the co-dehydrogenation of secondary alcohols enables lower reaction pressure and longer catalyst lifetime. Our work provides a sustainable and environmentally benign approach for producing 1,5-pentanediol from biomass-based furfural and its derivatives, which has potential applications in polymer synthesis and green chemistry.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Jia Deng,Weiguo Chen,Feng Wu,Yitao Dai,Dionysios D. Dionysiou,Li-Zhi Huang
Peroxymonosulfate (PMS)-based advanced oxidation processes have become promising water treatment technologies in recent years. The redox cycle between transitional metals in heterogeneous catalysis is essential for continuous activation of PMS and efficient removal of pollutants. In this work, we prepared Fe 3 O 4 using precipitation method and subsequently added Ni aqueous solution to synthesize Ni-Fe (hydr)oxides. Ni-Fe (hydr)oxides show efficient PMS activation ability, causing the degradation of 96.8 % trichloroethylene (TCE) after 40 min with the dosage of Fe, Ni and PMS at 0.2, 0.1 and 0.2 mM, respectively. The catalyst concentration normalized TCE degradation rate constant of Ni-Fe (hydr)oxides/PMS system reaches 1.48 L g −1 min −1 . Nonradical pathway is dominant at the initial stage of the reaction which generates high-valent metals, SO 5 • − and indirectly produces 1 O 2 . 1 O 2 and dissolved O 2 together participate in the O 2 cycling, •OH generation, and electron transfer involving the reduction of trivalent metals. Divalent metals react with PMS to generate strong oxidative •OH and SO 4 • − through radical pathway in later stage. TCE is degraded and dechlorinated by multiple reactive species in Ni-Fe (hydr)oxides/PMS system. The optimum Ni/Fe ratio of catalysts under the studied conditions was 0.50. Ni-Fe (hydr)oxides show high reactivity and stability in real water matrices, demonstrating Ni-Fe (hydr)oxides are promising catalysts for PMS activation to degrade pollutants in contaminated water.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Jinxiao Ba,Wei Cai,Yifan Chen,Li Lin,Yule Huang,Xianghai Yu,Yihua Wang,Chengqun Xu,Donghua Fan,Lisong Yin
In this work, pure and homogeneous Ni incorporated CdS photocatalyst was prepared by vulcanization of ZIF material synthesized from Cd/Ni salt by solvothermal method . The prepared pure CdS photocatalysts by the vulcanization of ZIF material exhibits better catalytic activity due to its larger specific surface area. The introduction of Ni can further improve the hydrogen production activity. The effect of Ni incorporating amount and annealing temperature on the hydrogen production activity of CdS photocatalyst was researched systematically. The photocatalytic activity at 10 % Ni incorporated CdS sample is greatly enhanced after annealing at 700 °C, which is attributed to the effective doping of Ni into the CdS lattice by annealing. The average hydrogen evolution rate is 1644.6 μmol/g/h, which adds up to about 119 times that of normal CdS. The current research provides a simple and effective method for improving the photocatalytic activity of CdS.
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ACS Catalysis
·
2023
·
IF 12.9
Wei Lin,Yi Chen,Yuexing Zhang,Yongsheng Zhang,Jianshe Wang,Liucheng Wang,Chunbao Charles Xu,Renfeng Nie
Ni–ReOx bimetallic catalysts (Ni–ReOx/TiO2) were prepared through a successive impregnation method, which is extremely active in furfural (FAL) hydrogenation to tetrahydrofurfuryl alcohol (THFOL) under mild reaction conditions. For instance, high FAL initial reaction rate (439.4 mmol/g-Ni/h) and THFOL formation rate (80.4 mmol/g-Ni/h) were achieved over Ni–5ReOx/TiO2, which are 13.2 and 6.6 times higher than those of Ni/TiO2, respectively. The unique catalyst reactivity derives from rich Lewis acidic ReOx and intimate electron interaction of ReOx with Ni NPs. Kinetic studies reveal that ReOx decoration decreases the activation barrier of −C═O hydrogenation other than the furan ring. Mechanism studies show that ReOx has a good affinity for C═O and H2 and favors hydrogen spillover and C═O bond activation on Ni, thus reinforcing the synergistic effect of Ni and ReOx. This catalyst is versatile for various furan aldehydes and is relatively stable for 5 times recycling, showing relative potential for industrial application.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Shixiang Xue,Tong Zhou,Pan Wu,Liang Zhao,Yanli Nan,Mingtao Qiao,Wanying Lei
Exploring high-efficient, earth-abundant and stable electrocatalyst for oxygen evolution reaction (OER) is of vital importance for large-scale implementation of energy converting and storing. Thus, we fabricated a free-standing hierarchical heterostructure electrode of Ni 0.85 Se@CoFe LDH/NF via a rational combination of hydrothermal, selenization and electrodeposition process, among which the ultrathin CoFe LDH nanosheets intimately assembled onto the vertical aligned Ni 0.85 Se nanosheets supported on Ni foam. The constructed core-shell nanosheet arrays hold the plentiful hetero-interfaces and intimate interactions through metal-oxygen bonds between two individuals, which guarantee the fast OER kinetic processes. Additionally, CoFe LDH with crystalline/amorphous hybrid structure favors providing more reaction sites. Remarkably, the optimal Ni 0.85 Se@CoFe LDH/NF binary composites possess outstanding OER activity with a low overpotential of ∼223 and 280 mV at 10 mA cm −2 and 100 mA cm −2 in alkaline solution as well as good durability. This research offers an alternative approach for improving electrocatalytic water splitting through constructing 3D hierarchical heterostructures.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Shunfa Zhou,Guoli Zheng,Feng Ji,Jiatang Wang,Zhao Liu,Jiawei shi,Jing Li,Yang Hu,Chengwei Deng,Liyuan Fan,Weiwei Cai
Excellent porosity and accessibility are key requirements during carbon-based materials design for energy conversion applications. Herein, a Ni-based porous supramolecular framework with graphite-like morphology (Ni-SOF) was rationally designed as a carbon precursor. Ultrathin carbon nanosheets dispersed with Ni nanoparticles and Ni-N x sites (Ni@NiN x -N-C) were obtained via in-situ exfoliation during pyrolysis. Due to the hetero-porous structure succeeding from Ni-SOF, the Ni@NiN x -N-C catalyst showed outstanding bifunctional oxygen electrocatalytic activity with a narrow gap of 0.69 V between potential to deliver 10 mA cm −2 oxygen evolution and half-wave potential of oxygen reduction reaction, which even surpassed the Pt/C + IrO 2 pair. Therefore, the corresponding zinc-air battery exhibited excellent power output and stability. The multiple Ni-based active sites, the unique 2D structure with a high graphitization degree and large specific surface area synergistically contributed to the excellent bifunctional electrocatalytic activity of Ni@NiN x -N-C. This work provided a novel viewpoint for the development of carbon-based electrocatalyst.
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