JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Yun Tian,Mengqiao Gao,Zhiyang Tang,Fukun Li,Qiang Zeng,Jinxing Long,Xuehui Li
Conversion of lignin to valuable chemicals without external hydrogen presents a significative but challengeable endeavor. Herein, an efficient approach has been proposed for the lignin hydrogenolysis with in-situ hydrogen in the presence of Ni nanoparticles nested in layered double oxides (LDOs). 84.4 % conversion of lignin was achieved over 30Ni-Mg 3 Al-LDOs, affording a 21.3 % yield of monomers, and 38.0 % of which was identified as 4-ethylphenol. Catalyst characterizations revealed that this excellent performance of lignin conversion should be ascribed to the highly dispersed Ni nanoparticles, strong interfacial interactions between Ni and LDOs, and suitable basicity of catalysts. Furthermore, the roles of the solvent (1,4-dioxane aqueous solution) and the lignin methoxyl groups as hydrogen resources were distinguished, and the former acted as an initial hydrogen to promote lignin depolymerization, and the latter was responsible for the high yield of 4-ethylphenol. In addition, a plausible reaction pathway for lignin hydrogenolysis has been proposed.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Shu-Xiang Xiang,Jin-Peng Wang,Su Gao,Zhan-Kuo Guo,Hui-Lin Jiang,Bao-Xia Dong,Yun-Lei Teng
The CH 4 yield over dual functional materials (DFMs) remains low and requires further improvement. In this work, we first examined the influence of Mn on the performance of the Ni-CaO/γ-Al 2 O 3 DFM for CO 2 capture and in situ methanation. Our results showed that the MnNi-DFM-3 (MnNi-CaO/γ-Al 2 O 3 DFM) exhibited the best performance at 350 °C, with a CH 4 yield of 0.56 mmol/g which is 4 times higher than that of the Ni-DFM-1 (Ni-CaO/γ-Al 2 O 3 DFM) (0.14 mmol/g). Nanoscale characterization revealed that highly scattered Mn 3 O 4 acted as a barrier preventing the agglomeration of Ni-based catalysts. Furthermore, our density functional theory (DFT) analysis demonstrated that the introduction of Mn enhanced the activation of CO 2 , promoted the dissociation of H 2 and intermediates, and reduced the activation energy needed to produce carboxylic acid intermediates on the Ni catalyst. The prepared MnNi-DFM is promising to be a cheap efficient material for CO 2 capture and in situ methanation. This work opens up a new pathway for enhancing the performance of DFMs using inexpensive transition metals.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zifan Wu,Yacong Deng,Fengyu Tian,Yidi Wang,Na Fan,Guangzheng Sun,Yichuan Li,Yuan Pan,Bin Liu,Bin Dong,Han Hu,Yongming Chai
During the fermentation of straw to produce bioethanol, enzymatic hydrolysis lignin (EHL) is generated in significant quantities, which retains the original structure of lignin and thus exhibits a great potential for the production of monophenols. Herein, we fabricated a highly dispersed Ni-Co alloy catalyst loaded on N-doped biochar (10Ni-3Co/NAC) by a deposition precipitation method, which could completely convert α-O-4, β-O-4, and 4-O-5 lignin model compounds into monomers under mild conditions. 10Ni-3Co/NAC significantly catalyzed the hydrocracking of EHL in water at 220 °C under 3 MPa of initial hydrogen pressure for 8h, achieving a total monophenol yield of 42.8 wt% and a high 2,6-dimethoxy-4-propylphenol proportion (48.5 %). The study results suggest that 10Ni-3Co/NAC possesses high adsorption and activation capacity for oxygen-containing substrates, and the interspecies electron transfer within Ni-Co alloys in 10Ni-3Co/NAC facilitates the formation of dissociated active hydrogen, which attacks the C-O group in EHL leading in the highly selective cleavage of the C-O bond to produce monophenols.
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高影响因子
FUEL
·
2025
·
IF 7.5
Han Yang,Jing Li,Qiang Chang,Qun-chao Zhao,Meng-na Zhang,Huan-jiang Wang,Cheng-hua Zhang,Fei Wang,Xiao-dong Wen
The catalytic production of hydrogen (H 2 ) through the decomposition of ammonia (NH 3 ) using non-noble metal catalysts with small nanoparticles and high electronegativity at elevated loadings is considered a promising approach for efficient on-site H 2 production. However, excessive loading may undermine the interactions between the metal and the support, resulting in sintering and deactivation of the active components in catalysts at high temperatures. Herein, a layered nickel (Ni) phyllosilicate with varying Ni content was successfully synthesized using amorphous silicon nitride (Si 3 N 4 ) as the silica source through a straightforward deposition–precipitation method. The characterization of Si 3 N 4 -derived Ni phyllosilicate indicates that it is more thermally stable than fumed SiO 2 -derived Ni phyllosilicate when used as a catalyst precursor. Upon 700 °C reduction of Si 3 N 4 -derived Ni phyllosilicate containing 20.0 wt% Ni, small-sized (4.2 nm) and highly dispersion Ni nanoparticles were formed and embedded within the unreduced Ni Phyllosilicate matrix (NiPS-Red700). More importantly, the NiPS-Red700 is presented for efficient catalytic activity and stability for NH 3 decomposition at 700 °C with a gas hourly space velocity (GHSV) of 60,000 mL/g cat /h, being much superior to Ni/SiO 2 catalysts prepared from the same synthesis method. The exceptional catalytic performance of NiPS-Red700 arises from the synergy of highly dispersed and electron-rich Ni nanoparticles, which facilitate the dissociation of the N–H bond and promote the combination of surface N* for N 2 associative desorption, ultimately enhancing the decomposition of NH 3 .
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Changzhou Chen,Xialin Ji,Yongzhi Xiong,Jianchun Jiang
Exploring an advanced catalytic strategy for the high value utilization of lignin derived chemicals into value-added aromatics has attracted tremendous sights for green manufacturing. In this paper, a series of bifunctional 3D rod-shaped mesoporous NiCe metal–organic framework catalysts coupling with hydrogen-donner solvent were reported for the hydrodeoxygenation of vanillin to obtain 2-methoxy-4-methylphenol. Under the optimal conditions, 3Ni-Ce/C catalyst realized the highest conversion of vanillin (>95.0 %) and selectivity of 81.4 % in the absence of additional hydrogen pressure. The characterization results indicated that the interaction of metallic Ni and CeO 2 promoted the generation of Ni-CeO 2-x interface and oxygen vacancies (Ov), which could efficiently adsorb and activate aldehyde group of vanillin to obtain reactive intermediates. And then metallic Ni sites activated the hydrogen-donner solvent to form adsorbed H atoms, which then spilled over to the adjacent Ov to stabilized reactive intermediates. Whereafter, bifunctional 3D rod-shaped mesoporous NiCe metal–organic framework catalysts achieved the hydrodeoxygenation upgrading of vanillin to obtain 2-methoxy-4-methylphenol. Density functional theory (DFT) calculations further revealed that the synergistic effect of Ni-CeO 2 and oxygen vacancies promoted the activation and dissociation of aldehyde group bond in vanillin, enhanced the ability of protonation hydrogenolysis. Additionally, 3Ni-Ce/C catalyst displayed robust activity for no less than four recycles, which provided a feasible method for the build of simultaneous utilization of lignin derivates to value-added fuels and chemicals.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Ke Lu,Yihao Xu,Hao Yuan,Jianping Liang,Hongli Wang,Jie Zhang,Yinong Li,Dezheng Yang
The design of efficient reaction units and the use of efficient catalysts for green and non-polluting ammonia synthesis is an important and challenging issue. In this paper, we design a high-efficiency reaction device, a coaxial double dielectric barrier discharge plasma reactor, which produces a more uniform plasma discharge during operation, changes the discharge characteristics, promotes the physicochemical reactions of ammonia synthesis, improves the efficiency of ammonia production, and reduces the energy consumption. The use of transition metal Ni and its metal oxide NiO loaded on the carrier as catalysts. The catalyst was comprehensively characterized by X-ray photoelectron spectroscopy, X-ray diffraction, and scanning electron microscope. The reaction mechanism of plasma-catalyzed ammonia synthesis was studied in detail by combining discharge characteristics, optical emission spectroscopy, and catalyst characterization. The reaction conditions and discharge parameters of the dielectric barrier discharge plasma reactor were optimized, which greatly improved the energy efficiency and synthesis rate, which could reach 1002 μmol g −1 h −1 under the optimal conditions. Based on the experimental results, we analyzed how different conditions and parameters affect the reaction of ammonia synthesis.
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高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2024
·
IF 5.6
Xialin Ji,Xiaoke Tian,Mengqing Zhou,Changzhou Chen,Jianchun Jiang
In this study, different kinds of lignin, including enzymatic hydrolysis of lignin (EHL), alkaline lignin (AL), kraft lignin (KL) and sodium lignosulfonate (LS) were investigated as precursor to prepare Ni@BTC@X (X= EHL, AL, KL, LS) catalysts using a traditional hydrothermal method with Ni-MOF for HDO upgrading of lignin derivative vanillin (VAN) to generate high value chemical 2-methoxy-4-methylphenol (MMP). The catalytic performance of these catalysts was investigated under different reaction conditions, and it was explored that the conversion of VAN was close to 100 % and the MMP yield was close to 90 % under the optimal conditions (Ni@BTC@LS catalyst, 220 ℃, 4 h, isopropanol, 2 MPa N 2 ). Various physical-chemical characterization results verified that the effects of active sites Ni, porous structure of lignin biochar support and electronic properties of the catalysts played a significiant role in HDO of lignin derived VAN. Additionally, synergistic effect of the highly homogeneously dispersed oxygen vacancies and acidic sites also promoted the VAN conversion efficiency. This work developed a strategy combing the advantages of MOFs and biomass derived substrates for manufacturing novel lignin/MOFs materials in the catalytic field.
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高影响因子
CHEMOSPHERE
·
2024
·
IF 8.1
Bingnan Zhou,Bo Fan,Zhimin Gong,Shuai Shao,Dongmei Zhou,Shixiang Gao
The excessive usage and emissions of triclosan (TCS) pose a serious threat to aquatic environments. Iron-based bimetallic particles (Pd/Fe, Ni/Fe, and Cu/Fe, etc.) were widely used for the degradation of chlorophenol pollutants. This study proposed a novel synthesis method for the preparation of Ni/Fe bimetallic particles (Ni-Fe bm ) by ball milling microscale zero valent iron ZVI (mZVI) and NiSO 4 . Ball-milling conditions such as ball-milling time, ball-milling speed and ball-to-powder ratio were optimized to prepare high activity Ni-Fe bm bimetallic particles. During the ball-milling process, Ni 2+ was reduced to Ni 0 and formed a coupled structure with ZVI. The amount of Ni 0 on ZVI significantly affected the activity of Ni-Fe bm bimetallic particles. The highest activity Ni-Fe bm bimetallic particles with Ni/Fe ratio of 0.03 were synthesized under optimized conditions, which could remove 86.56% of TCS (10 μM) in aerobic aqueous solution within 60 min. In addition, higher particle dosage, lower pH condition and higher reaction temperature were more conducive for TCS degradation. The higher corrosion current and lower electron transfer impedance of Ni-Fe bm bimetallic particles were the main reasons for its high activity. The hydrogen atom (•H) on the surface of Ni-Fe bm bimetallic particles was mainly contributed to the removal of TCS, as reductive transformation products of TCS were detected by LC-TOF-MS. Notably, a small amount of oxidation products were discovered. The total dechlorination rate of TCS was calculated to be 39.67%. After eight reaction cycles, the residual Ni-Fe bm bimetallic particles could still degrade 28.34% of TCS within 6 h. Low Ni 2+ leaching during reaction indicated that Ni-Fe bm bimetallic particles did not pose potential environmental risks. The prepared environmental-friendly Ni-Fe bm bimetallic particles with high activity have great potential in the degradation of other chlorinated organic compounds in wastewater.
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PubMed
高影响因子
CHEMOSPHERE
·
2018
·
IF 4.427
Zilong Zhao,Zekun Liu,Hongjie Wang,Wenyi Dong,Wei Wang
Treatment of Ni-EDTA in industrial nickel plating effluents was investigated by integrated application of Fenton and ozone-based oxidation processes. Determination of integrated sequence found that Fenton oxidation presented higher apparent kinetic rate constant of Ni-EDTA oxidation and capacity for contamination load than ozone-based oxidation process, the latter, however, was favorable to guarantee the further mineralization of organic substances, especially at a low concentration. Serial-connection mode of two oxidation processes was appraised, Fenton effluent after treated by hydroxide precipitation and filtration negatively affected the overall performance of the sequential system, as evidenced by the removal efficiencies of Ni 2+ and TOC dropping from 99.8% to 98.7%, and from 74.8% to 66.6%, respectively. As a comparison, O 3 /Fe 2+ oxidation process was proved to be more effective than other processes (e.g. O 3 -Fe 2+ , O 3 /H 2 O 2 /Fe 2+ , O 3 /H 2 O 2 -Fe 2+ ), and the final effluent Ni 2+ concentration could satisfied the discharge standard (<0.1 mg L −1 , China) under the optimal conditions (H 2 O 2 dosage of 1.0 mL L −1 , Fe 2+ : H 2 O 2 mole ratio of 1.46, and reaction time of 10 min for Fenton reaction , initial influent pH of 3.0, O 3 dosage of 252 mg L −1 , Fe 2+ of 150 mg L −1 , and reaction time of 30 min for O 3 /Fe 2+ oxidation). Furthermore, pilot-scale test was carried out to study the practical treatability towards the real nickel plating effluent, revealing the effective removal of some other co-existence contaminations. And Fenton reaction has contributed most, with the percentage ranging from 72.41% to 93.76%. The economic cost advantage made it a promising alternative to the continuous Fenton oxidation.
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高影响因子
WATER AIR AND SOIL POLLUTION
·
2018
·Vol. 229
·期 3
·1-10
·
IF 1.769
Yi Yunqiang,Wu Juan,Wei Yufen,Fang Zhanqiang,Gong Yanyan,Zhao Dongye
Ni/Fe bimetallic nanoparticles have been widely used as strong reductants to degrade organic pollutants. Synthesis parameters of Ni/Fe nanoparticles can directly affect their characteristics and reactivity. In this study, Ni/Fe nanoparticles were prepared at different synthesis conditions, namely, synthesizing temperature, stirring rate, washing solutions, and preparation methods (post-coated and co-reducted Ni/Fe nanoparticles), and investigated their effectiveness of decabrominated diphenyl ether (BDE209) degradation. The results showed that the successive order of factors affecting the kinetics constant of Ni/Fe nanoparticles for the removal of decabrominated diphenyl ether (BDE209) were preparation methods, washing solutions, stirring rate, and synthesis temperature. It should be noted that the kinetics constants of post-coated Ni/Fe nanoparticles for removal of BDE209 was 0.049 min −1 , which was 14 times higher than that of co-reducted Ni/Fe nanoparticles. Moreover, the most remarkable influence on the particle size of Ni/Fe nanoparticles was the stirring rate, others synthesis conditions are mentioned in the following order: washing solutions > preparation methods > synthesis temperature. Interestingly, the effects of synthesis condition on the crystalline structure of Ni/Fe were weak. The results may facilitate more effective application of Ni/Fe nanoparticles for degradation of BDE209.
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高影响因子
FUEL PROCESSING TECHNOLOGY
·
2018
·
IF 3.956
Limo He,Song Hu,Long Jiang,Guang Liao,Xiaofang Chen,Hengda Han,Lingfeng Xiao,Qiangqiang Ren,Yi Wang,Sheng Su,Jun Xiang
The effects of catalyst supports (γ-Al 2 O 3 and α-Al 2 O 3 ) on hydrogen yield and carbon nanotubes formation were studied during steam reforming of toluene over Ni-based catalysts. Hydrogen yield and CNTs quality over Ni/γ-Al 2 O 3 were better than those over Ni/α-Al 2 O 3 at S/C ratio of 1 due to the high Ni dispersion of Ni/γ-Al 2 O 3 . With the increasing of steam addition, CNTs production remarkably increased over Ni/α-Al 2 O 3 , while it decreased over Ni/γ-Al 2 O 3 . The CNTs on Ni/γ-Al 2 O 3 were corroded at S/C ratio of 3 by excess steam. Toluene conversion and hydrogen yield over Ni/α-Al 2 O 3 were significantly larger than those over Ni/γ-Al 2 O 3 , which was attributed to the different effects of CNTs on catalytic activity . The strong interaction between Ni particle and γ-Al 2 O 3 led to the base-growth mechanism of CNTs on Ni/γ-Al 2 O 3 in which Ni particles located at the bottom of CNTs, thus the growth of CNTs covered Ni active sites and decreased catalytic activity of Ni/γ-Al 2 O 3 . By contrast, owing to weak interaction, CNTs grown on Ni/α-Al 2 O 3 followed tip-growth mechanism that would increase Ni dispersion and promote reforming reaction .
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xing Yi,Yan Wang,Zongpeng Zou,Yuan He,Li Lv,Wenxiang Tang,Tao Zhang,Shengwei Tang
The microreactor coupled mini-channel microdroplets extraction and separation technology (MES) was developed by adding polyvinyl alcohol (PVA) into microdroplets, realizing the controllable synthesis of a series of mono-component and multi-component metal oxide nano particles (MONPs). A double-layer surfactant structure composed of Span20 (oil phase surfactant) and PVA (water phase surfactant) was designed as a barrier to intercept and collect the precipitated salt at the microdroplet interface, the addition of PVA reduces the loss of salt components during the extraction process from 41.7 wt% to 1.1 wt%. The size control of mono-component MONPs (CuO, Co 3 O 4 , and NiO) was achieved using MES method. Furthermore, in the application direction of preparing multi-component MONPs, the advantages of MES in preparing multi-component catalysts (Ni/CeO 2 ) were verified. TEM, XRD, H 2 -TPR, CO 2 -TPD, XPS, BET et al. characterizations have shown that Ni entered the lattice of CeO 2 during precipitation to form a Ni-O-Ce solid solution and was therefore highly dispersed in CeO 2 . Ni/CeO 2 -MES showed high CO 2 conversion and CO selectivity in reverse water gas shift (RWGS) testing compared to Ni/CeO 2 catalysts prepared by impregnation method which has excellent thermal stability and can maintain over 99 % CO selectivity even after 50 h of reaction at 600 °C. The MES method was proved to be an efficient synthesis technology for MONPs and can be extended to a variety of metal oxides catalysts.
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