ACS Applied Materials & Interfaces
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2022
·
IF 10.383
Chao Miao,Shumei Chen,Kaixuan Shang,Lixing Liang,Jing Ouyang
The dry reforming of methane (DRM) is a new potential technology that converts two major greenhouse gases into useful chemical feedstocks. The main challenge faced by this process is maintaining the catalyst with high catalytic activity and long-term stability. Here, a simple and effective preparation route for the synthesis of functional nanomolecular sieve catalysts (NiRuxCZZ5) from kaolinite tailings was developed for dry reforming of methane with CO2. The silica monoliths with flower-like spherical and micropore structures (ZSM-5) were prepared by crystal growth method, and the metal components were loaded by ultrasonic-assisted impregnation method. The NiRu0.5CZZ5 catalyst exhibited excellent catalytic performance (maxmium CO2 and CH4 conversions up to 100 and 95.6%, respectively) and very good stability (up to 100h). The interfacial confinement and the strong support interaction are principally responsible for the excellent catalytic activity of the catalyst. The in situ DRIFTS was used to elucidate the possible carbon conversion steps, and stable surface intermediates were also identified.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Junjing Li,Shumin Ma,Ziyan Qi,Jing Ding,Menghua Yin,Bin Zhao,Zhaohui Zhang,Yu Wang,Hongwei Zhang,Liang Wang,Dionysios D. Dionysiou
To effectively improve the particle dispersion of the catalytic metal and catalytic activity of the palladium electrode, a new type of efficient Pd/NiFe-MOF/foam-Ni composite electrode was prepared. The results showed that the reaction rate constant of chloramphenicol (CAP) by Pd/NiFe-MOF/foam-Ni was three times that of Pd/foam-Ni. X-ray absorption fine structure (XAFS) results showed that palladium on Pd/NiFe-MOF/foam-Ni had a lower oxidation state than that on Pd/foam-Ni. The Pd nanoparticles were uniformly dispersed on the composite electrode and had a small particle size. The electrode had good resistance to sulfites and the electrocatalytic activity was hardly affected in the presence of Cl - , NO 3 - , HCO 3 - , CO 3 2- and Ca 2+ in wastewater. Besides, the introduction of nickel-iron bimetallic organic framework (NiFe-MOF) increased the electron density of Pd, improved the dispersion and electrochemical active surface area (ECSA) of Pd. The reaction pathway of CAP was proposed, and the ecotoxicity of CAP and its products was evaluated by the Ecological Structure Activity Relationships (ECOSAR) model. Combined experimental data and density functional theory (DFT) analysis enable us to propose the hydrodechlorination mechanism of CAP on the Pd/NiFe-MOF/foam-Ni electrode. The Pd/NiFe-MOF/foam-Ni composite electrode has good application prospects in the treatment of organic pollutants in wastewater and other environmental remediation applications.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Wenqing Du,Yongqian Zheng,Xueyi Liu,Jie Cheng,R. Chenna Krishna Reddy,Akif Zeb,Xiaoming Lin,Yifan Luo
Transition metal oxide anode materials have recently been losing their importance as advanced functional and smart materials due to early capacity decay and sluggish kinetics. In order to address this issue, vacancy engineering approach can be adapted, which can effectively manipulate the electronic structure of transition metal oxide (TMO)-based electrode materials. Herein, a series of MOF-derived oxygen-rich vacancy MFe 2 O 4 /C (M = Ni, Mn, Co) materials are synthesized on a large scale via solvothermal and subsequent calcination treatment for energy storage applications in lithium-ion batteries. All the synthesized O V -NFO (NiFe 2 O 4 ), O V -MFO (MnFe 2 O 4 ) and O V -CFO (CoFe 2 O 4 ) electrodes achieve excellent electrochemical performance, superior multiplier performance and incredible lithium-ion diffusion rate, which was found to be superior than their counterpart electrodes. The oxygen vacancy (O V ) enrichment contribution to higher conductivity was realized by experimental and density functional theory (DFT) calculations results, where it has been established that O V provides additional active sites, accelerates Li + diffusion and improves pseudocapacitive contribution. This vacancy-engineering strategy for modulating electronic structure and reaction kinetics enabled new ideas for the design and execution of other advanced transition metal-based electrode materials.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Feng Chen,Xinqi Zhu,Weilong Dai,Congcong Yao,Junchao Qian,Zhigang Chen,Chengbao Liu
The high nickel cathode LiNi 0.83 Co 0.06 Mn 0.06 Al 0.05 O 2 (combination of NCM and NCA) coated with the Li + conductor Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 in various mass fractions was prepared via using the typical sol-gel process. The LiNi 0.83 Co 0.06 Mn 0.06 Al 0.05 O 2 after the Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 covering demonstrated the similar crystal structure and particle morphology in comparison with the bare cathode. The electrochemical test results indicated the superior rate capabilities and cycling performances were acquired for the coated cathodes due to the presence of the Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 film on the surface of LiNi 0.83 Co 0.06 Mn 0.06 Al 0.05 O 2 . The 2 wt% Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 covered LiNi 0.83 Co 0.06 Mn 0.06 Al 0.05 O 2 exhibited the greatest electrochemical performance with a large cycle retention rate of 90.9% over 300 cycles at 45 °C, rate capacity of 139.8 mAh g −1 at 5 C current density, and a high capability of 126.5 mAh g −1 at − 30 °C, superior than those (80.9%, 99.8 mAh g −1 , 71.3mAh g −1 accordingly) of the bare cathode. In addition, the safety and environmental reliability tests of pouch batteries suggested the Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 film on the surface of cathode acted as a protective layer to promote the stability for application.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Manfen Liang,Yu Liu,Hong Huang,Lechen Diao,Jinglin Mu,Zhichao Miao,Jin Zhou,Shuping Zhuo
The electrochemical CO 2 reduction reaction (CO 2 RR) to CO is regarded as a potential way to relieve CO 2 level and produce value-added chemicals. However, most reported catalysts only possess high Faraday efficiency of CO (FE CO %) under a narrow potential range, and this shortage largely limits its ultimate practical viability. Herein, we develop a facile method to synthesize nickel encased by nitrogen-doped carbon nanotubes on carbon support (Ni@NCNT-C) catalyst for CO 2 RR. As for the important influence factors, the Ni content and treatment temperature are carefully controlled, and their influence on textural property and catalytic performance is investigated. The 0.1Ni@NCNT-C-800 catalyst provides a low overpotential (−0.27 V vs. RHE) and high FE CO % (∼100%). The CO partial current density can reach 230 mA cm −2 and the activity can be maintained over 40 h. More importantly, a wide potential range of 900 mV (−0.27 V to − 1.17 V vs. RHE) can be obtained when FE CO % is continuously maintained at nearly 100%. This work may provide a route to seek a robust catalyst for high-efficiency CO 2 RR over a wide potential range.
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ACS Omega
·
2022
·
IF 4.132
Xiaofeng Li,Xiaohui Liu,Jiamao Hao,Lijun Li,Yanfang Gao,Yousong Gu,Zhenzhu Cao,Jinrong Liu
A strong metal–support interaction (SMSI) type catalyst has been synthesized and applied to a molten hydroxide direct carbon fuel cell (MHDCFC) to enhance the reaction activity of the anode carbon fuel through the interaction between the metal Ni and the support CeO2. Two catalysts have been prepared by a direct precipitation method (denoted NiO@CeO2) and a hydrothermal method (denoted NiO-CeO2), which are reduced by H2 to obtain Ni@CeO2 and Ni-CeO2, respectively. X-ray photoelectron spectroscopy (XPS), Raman, and temperature-programmed hydrogen reduction (H2-TPR) analysis results show that there are obvious oxygen vacancies and a Ni-O-Ce interface structure in NiO-CeO2 and Ni-CeO2, which is induced by the interaction between Ni and CeO2. The calculation results of current density and power density show that the performance of the MHDCFC is significantly improved in the presence of Ni-CeO2. The function fitting curves of the logarithm of the reaction rate constant (ln k) and the reciprocal of the temperature (1/T) show that the slope of the curve is decreased significantly after the addition of Ni-CeO2. In combination with density functional theory (DFT), the anode carbon reaction path is simulated in the MHDCFC, and the calculation results show that the reaction energy for the anodic carbon to generate carbon dioxide is decreased by 1.03 eV in the presence of Ni-CeO2.
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高影响因子
JOURNAL OF FLUORESCENCE
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2022
·Vol. 32
·期 5
·1743-1754
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IF 2.525
Xu Ouwen,Wan Shuyu,Yang Jing,Song Hanyang,Dong Luzheng,Xia Ji,Zhu Xiashi
In this work, an “on-off-on” fluorescent probe based on Ni-MOF functionalized Nitrogen-doped carbon quantum dots (Ni-MOF-NCDs) was developed. Ni-MOF-NCDs was characterized by FT-IR, TEM, SEM, and XPS. The presence of Fe (III) will reduce the fluorescence intensity of Ni-MOF-NCDs and “turn off” the fluorescence signal at emission peak of 390 nm, while the signal can be “turn on” after the addition of ascorbic acid (AA). The Ni-MOF-NCDs was established as an “on-off-on” fluorescent probe for the detection of Fe (III) and AA with the linear ranges of 0.029-8.0 µg/mL and 0.263-18.0 µg/mL, respectively. The method has been successfully applied to the detection of water samples and foods with satisfactory recovery. The experimental results showed that Ni-MOF-NCDs not only had the fluorescence properties of NCDs, but also had the adsorption performance of Ni-MOF.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Yibin Zhu,Juwen Gu,Zan Huang,Hanlin Ding,Hongyan Xia,Songbai Qiu,Kang Xie
Recently, electrospinning technology has high-potential applications in the large-scale manufacturing of one-dimensional (1D) nano-catalytic functional materials . Herein, Ni nanoparticles embedded within highly N-doped carbon nanofibers (Ni@NCNFs) were fabricated using polyacrylamide (PAM) and nickel acetate (NiAc) aqueous solutions as precursors by electrospinning and subsequent carbonization for the first time. The as-prepared Ni@NCNFs were smoothly applied to the hydrogenation of quinoline toward 1,2,3,4-tetrahydroquinoline and manifested excellent catalytic performance with extremely high selectivity (99.0%) at full conversion (99.3%). The influence factors on the physicochemical properties were further studied, including the carbonization temperature, the PAM mass fractions and the mole ratios between PAM and NiAc (PMA/Ni). The present work demonstrated that electrospinning and carbonization could be potential technologies for manufacturing Ni@NCNFs as an outstanding catalyst for quinoline hydrogenation. Furthermore, PAM rich in nitrogen could serve as a new alternative electrospinning precursor for future applications.
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CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
Yuan Shu,Xuefeng Ma,Xiaolan Duan,Dandan Liu,Li Wang,Qiang Niu,Pengfei Zhang
Designing highly dispersed metal nanoparticles (NPs) working at high temperature reductive atmosphere remains a challenge, especially for non-noble metal NPs (e.g., Ni NPs). Here, a solid-state co-precipitate method was developed to prepare sintering-resistance Ni-ZnO catalyst. The catalyst featured as high Ni dispersion by this solid-state co-precipitate method in solid solution, and ∼ 6 nm Ni NPs were obtained even in a long-term reduction pre-treatment (500 °C, H 2 ). Interestingly, a well-established strong metal and support interaction (SMSI) effect of Ni-ZnO was observed during the reduction process. A thin ZnO overlay was clearly deposited on the Ni metal NPs, effectively tuning the geometry and electronic structure of the exposed Ni metallic sites. Combined with the evidence of CO-TPD, H 2 O-TPD, H 2 O-titration, and CO-H 2 O TPSR, the existence of Ni-ZnO SMSI strongly provides the unusual pathway of redox mechanism during water gas shift (WGS) reaction, avoiding the tendency of CO methanation reaction in traditional Ni-based catalytic systems.
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Catalysts
·
2022
·Vol. 12
·期 5
·460
·
IF 4.501
Yifan Zheng,Lijun Lu,Wei Chen,Anmin Zheng,Aiwen Lei,Abhishek Dutta Chowdhury
Global warming and rising waste content collectively accelerate the development of renewable-derived ‘low-carbon’ chemical technologies. Among all abundant renewables, marine-/food-waste-derived chitin, the only nitrogen-containing sustainable biomass, contains the uniqueN-acetylglucosamine units, which could be synthetically manipulated to a plethora of organonitrogen chemicals. Herein, we report the efficient one-step catalytic valorization of chitin toN-acylethanolamine over cost-effective Ni/CeO2-based materials, which interestingly demonstrate shape-based reactivity based on CeO2supports. In general, all three catalysts (Ni on cubic-, rod-, and polyhedral-shaped CeO2supports) were active for this reaction, but they differed in their catalytic efficiency and time-monitored reaction profiles. Herein, Ni on cubic-shaped CeO2delivered relatively better and stable catalytic performance, along with its rod-shaped counterpart, while the polyhedral CeO2-based material also delivered decent performance. Such interesting catalytic behavior has been corroborated by their physicochemical properties, as revealed by their characterization studies. Herein, to establish an appropriate structure-property-reactivity relationship, multimodal characterization techniques and control mechanistic experiments have been performed. This work demonstrates a concept to reduce the consumption of primary carbon resources and increase the utilization of secondary waste materials to facilitate a smooth transition from a linear economy (cf. cradle-to-grave model) to a circular economy (cf. cradle-to-cradle model).Keywords:chitin;waste valorization;heterogeneous catalysis;ceria;functionalization of C–C bonds
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FUEL
·
2022
·
IF 8.035
Xiuquan Li,Zhongqing Yang,Li Zhang,Ziqiang He,Yunfei Yan,Jingyu Ran,Zukhra C. Kadirova
The catalytic reaction of ethane with CO 2 promotes the value-added conversion of natural gas and the resource utilization of greenhouse gases. In this work, the CO 2 -assisted ethane dehydrogenation reaction characteristics on Fe 1.5 Ni 0.5 /ZrO 2 (M, T, Mix) catalyst with different crystal plane structure were studied through catalyst activity test, catalytic reaction kinetics study and catalyst characterization analysis. It is found that the exposed crystal faces of the ZrO 2 -supported catalyst has a significant effect on the CO 2 -assisted ethane oxidative dehydrogenation reaction. The monoclinic phase Fe 1.5 Ni 0.5 /ZrO 2 -M catalyst exhibits the largest conversion of ethane (21.8%) and CO 2 (25.2%) and the maximum selectivity to C 2 H 4 (80.5%). Monoclinic phase of ZrO 2 selectively exposes the ( −1 1 1) and (1 1 1) low-index surfaces with higher oxygen vacancy (O v ) density and stronger metal-support interaction, which leads to the formation of more Fe x Zr 1-x O 2 structures with high catalytic activity. The reductive oxygen vacancy O v and Fe 2+ -O-Zr 3+ sites promote the activation of CO 2 through the cleavage of C=O bond to supplement O* species. The O* species on the oxidative Fe 3+ -O-Zr 4+ site are captured and combined with H* species derived from the selective cleavage of ethane C–H bond to generate H 2 O.
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FUEL
·
2022
·
IF 8.035
Ming Jiang,Xiaopeng Chen,Linlin Wang,Jiezhen Liang,Xiaojie Wei,Weijian Nong
Lignin is the most abundant renewable aromatic resource in nature; thus, the development of an efficient and economical catalysts that can depolymerize lignin into value-added aromatic monomers is highly desirable. Here, we report a single-atom Ni catalyst ( x Ni/CeO 2 -S, where x represents the Ni loading), in which the single-atom Ni sites are anchored to the oxygen vacancies on CeO 2 nanospheres, for the conversion of cellulolytic enzyme lignin (CEL) via depolymerization and hydrodeoxygenation. The 1.0Ni/CeO 2 -S catalyst performed the best, achieving a lignin oil (LO) and maximum monomer yield of 84.3 wt% and 32.6 wt%, respectively; a higher heat value of 31.64 MJ/Kg is achieved for LO compared to 23.03 MJ/Kg for CEL. Thus, single-atom nickel catalyst exhibited excellent activity and stability in promoting the depolymerization of lignin. These results validate the viability of single-atom metal catalysts for the conversion of lignin resources.
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