LANGMUIR
·
2026
·
IF 4.4
Bihui An,Mingkun Wu,Haoran You,Chenhao Zhang,Mengkui Tian
Electrochemical conversion of carbon dioxide (CO2) into syngas is an effective strategy for mitigating global warming and enabling carbon circularity. However, achieving a tunable and stable H2/CO ratio remains challenging due to the competitive adsorption and reaction kinetics of CO2 reduction and hydrogen evolution. Herein, a metal–organic framework-derived pyrolysis strategy constructs CuNi bimetallic nanoclusters on nitrogen-doped carbon (CuNi–NC), where Cu–Ni electronic interactions enable site-specific regulation of surface adsorption. The optimized Cu1Ni1–NC catalyst achieves a high FECO of 93.3% and a CO partial current density of −25.82 mA cm–2, with excellent stability over 28 h. Across a broad potential window from −0.51 to −0.81 V (vs RHE), CO-rich syngas with an H2/CO ratio around 0.37 is consistently produced. Furthermore, the syngas composition can be tuned by modulating the Cu/Ni ratio and applied potential, altering the relative contribution of CuNi active sites differing in electronic structure. Combined in situ attenuated total reflection Fourier transform infrared spectroscopy and density functional theory calculations reveal that Cu–Ni electronic synergy induces site-specific electronic modulation, optimizing the d-band center to stabilize *COOH intermediates and promote selective CO2-to-CO conversion. This work establishes a Cu–Ni bimetallic catalytic system for tunable syngas production and provides mechanistic insight into site-specific adsorption driven by electronic synergy.
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DOI
PubMed
高影响因子
JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
·
2022
·
IF 4.383
Jingrong Wang,Zhihua Gao,Pengquan Yan,Yaxing Shen,Rui Yang,Zhijun Zuo,Wei Huang
CuO with a large microcrystalline differentiation was prepared by hydrothermal method , and the activity of the CuZnAl catalysts prepared by combining CuO with ZnAl was tested in the CO hydrogenation reaction. The effect of Cu species crystallite size on catalytic structure and performance was revealed. The experimental results show that CuO crystallite grow with the raising of hydrothermal temperature. When the hydrothermal temperature was 130 °C, CZA-130 exhibited the stable crystallite size of Cu species, high Cu/Zn molar ratio, and strong interaction between copper and zinc oxide, so the selectivity of total alcohol could reach up to 71.39%. Moreover, the ratio of C 2+ OH in the alcohol product is positively correlated with higher ratio of Cu + /Cu 0 and total number of alkalis, which are related to the ability of growing carbon chain.
研究领域:
化学工程
·
催化科学
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DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2020
·
IF 6.551
Mi Yan,Hongcai Su,Zhihao Zhou,Dwi Hantoko,Jianyong Liu,Jingyi Wang,Runpei Wang,Ekkachai Kanchanatip
The effluent of food waste (FWE) is generated during food waste treatment process. It contains high organic matter content and is difficult to be efficiently treated. In this study, the sample was collected from a 200 t/d food waste treatment center in Hangzhou, China. Subcritical and supercritical water gasification were employed to decompose and convert FWE into energy. The effects of reaction temperature (300–500 °C), residence time (20–70 min) and activated carbon loading (0.5–3.5 wt%) on syngas production and the remaining pollutants in liquid residue were investigated. It was found that higher reaction temperature and longer residence time favored gasification and pollutant decomposition, resulting in higher H 2 production and gasification efficiencies. It is noteworthy that the NH 3 -N was difficult to be converted and removed under current experimental conditions. The addition of activated carbon was found to increase the gasification efficiency. The highest total gas yield, H 2 yield, carbon conversion efficiency, gasification efficiency, total organic carbon removal efficiency and chemical oxygen demand removal efficiency were obtained from gasification at 500 °C for 70 min with 3.5 wt% activated carbon.
研究领域:
环境科学
·
能源工程
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DOI
高影响因子
Sustainable Energy & Fuels
·
2023
·
IF 5.6
Haowen Chen,Junwei Zhang,Kang Wang,Xitao Wang
In this work, a self-supported electrode based on porous carbon sheets was prepared by a high-temperature calcination of a phenolic resin using hexamethylenetetramine as a nitrogen source and curing agent and KCl salt templates as pore-forming agents, and it was tested for the electrocatalytic reduction of CO2 to syngas. The effects of the KCl addition amount on the morphology, pore structure, and electrocatalytic activity of the self-supported electrodes for CO2 reduction were also investigated. The results indicated that the amount of KCl has significant impacts on the morphology, pore structure, N-containing species and electrochemical properties of carbon materials. Specifically, the electrode with a 40% KCl content had a maximum surface area of 71.29 m2 g−1, a medium pore size of 22.47 nm, and a CO Faraday efficiency of 48% at −1.2 V vs. Ag/AgCl with a current density of 10 mA cm−2. Specifically, the H2/CO molar ratio could be adjusted from 1.09 to 3.38 by changing the applied potential. The superior electrocatalytic performance is attributed to the high strength, large specific surface area, and suitable pore structure of the material. The high strength ensures a stable and sustainable reaction, the large specific surface area fully exposes the reactive active sites, and the suitable pore structure promotes the effective adsorption of reactant CO2. The porous carbon sheet self-supported electrode designed in this experiment overcomes the disadvantages of expensive and short-lived precious metal catalysts and the need for adhesives in powder catalysts, providing a new strategy for the electrocatalytic conversion of CO2 into ideal products at low potentials.
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 30
·14142-14156
·
IF 3.3
Songyuan Hao,Wenbo Luo,Yaming Kang,Sen Fu,Hong Yuan
Syngas production from waste cooking oil (WCO) based on reforming with CO2 would allow the utilization of both resources. However, the catalysts used for reforming reactions (700–1000 °C) are prone to deactivation. In this work, La1−xSrxNiO3 (x = 0.1, 0.2) perovskites were prepared as catalyst precursors, then reduced and used for CO2 reforming of a waste cooking oil model compound (WCOMC). These materials exhibited stable catalytic activity during the reaction, attributed to the highly dispersed Ni0 nanoparticles on the La2O3 support and strong interactions between the metal and support. At 800 °C, the deposited amount of carbon on these catalysts decreased with increasing quantity of Sr doping into the A site of LaNiO3 and the syngas had a H2/CO ratio of 0.77. The present Sr-doped catalysts promoted the surface adsorption of oxygen along with the activation of C–H bonds. Most importantly, these materials strongly adsorbed CO2 and facilitated the conversion of carbon deposition to gaseous products.
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高影响因子
FUEL
·
2019
·
IF 5.128
Haimiao Yu,Yang Liu,Jiecheng Liu,Dezhen Chen
The study aims to evaluate the catalytic potential of a Ni-based catalyst supported by magnesium slag (MS) for catalytic reforming of pyrolysis volatiles from pine sawdust. The catalysts were prepared by a wet impregnation method. The effects of different parameters (Ni loading content, calcination/catalytic bed temperature and steam to carbon (S/C) ratio) on the catalytic performance were investigated. In addition, tar cracking capability and coke deposition resistance of Ni/MS catalyst and Ni/γ-Al 2 O 3 catalyst were explored under different calcination/catalytic bed temperatures. The catalysts were characterized by BET, XRD, SEM, TEM, TPO and Raman spectroscopy. The Ni/MS catalyst exhibited excellent catalytic reactivity as well as thermal stability. The best tar conversion (95.69%) and the highest hydrogen yield of 38.9 mmol/g biomass were obtained over Ni/MS catalyst under the conditions of Ni loading content = 3%, calcination/catalytic bed temperature = 800 °C, and S/C = 0.5. The interactions among Ni, Fe, Ca, and Mg formed multiple active centers (e.g., Ca 2 Fe 2 O 5 , (Ni, Mg) O solid solution and NiFe 2 O 4 ) in the catalyst to show synergistic catalysis effects, thereby jointly improving catalyst activity and coke deposition resistance. Furthermore, both amorphous carbon and graphitic carbon were formed on the used catalysts and the D/G ratio (the relative intensity ratio between the D and G bands) was positively correlated with the catalytic activity.
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高影响因子
ChemCatChem
·
2018
·Vol. 10
·期 20
·4689-4698
·
IF 4.674
Yan Liu,Ye Wu,Zarina Akhtamberdinova,Xiaoping Chen,Guodong Jiang,Dong Liu
Graphical High fives ! The catalyst 5Ni-5Ce exhibits the best catalytic performance in the dry reforming of shale gas and CO 2 . The introduction of Ce creates strong interaction between Ni and Ce, which enhances the electron transfer between them. And the substitution of Ni for Ce produces oxygen vacancies and defects, which can accelerate the adsorption and activation of the reactant gases molecule, further promoting the reaction. The dry reforming of shale gas (methane and ethane with an average ratio of 4 : 1) with carbon dioxide (DRS) is considered to be a promising way to produce syngas, which widens the utilization of shale gas and mitigates carbon dioxide emission. In this paper, Ce modified Ni-based catalysts were developed and the corresponding catalytic performances for DRS were investigated with a fixed bed reactor. Results showed that the catalyst containing 5 wt% of Ni and 5 wt% of Ce performed a best catalytic effect, including the selectivity of syngas and the carbon resistance performance, which is due to the good metal dispersion, strong interaction between Ni and Ce, and the formation of Ni-CeO x solid solution. The electron transfer between Ni and Ce, substitution of Ni for Ce, and the sequential oxygen vacancies or defects, play significant roles in activating CH 4 , C 2 H 6 and CO 2 . The conversion of reactant gas increased with temperature, while the selectivity of syngas is little affected with temperature. In addition, the desired catalyst containing 5 wt% of Ni and 5 wt% of Ce showed good stability in the long-time operation, which indicates that the Ce modified Ni-based catalyst is a promising one for the dry reforming of shale gas.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2022
·
IF 12.92
Zhaopeng Liu,Youming Ni,Zhongpan Hu,Yi Fu,Xudong Fang,Qike Jiang,Zhiyang Chen,Wenliang Zhu,Zhongmin Liu
The utilization of metal oxide-zeolite catalysts in the syngas-to-olefin reaction is a promising strategy for producing C 2 –C 4 olefins from non-petroleum resources. However, the effect of the crystal phase of metal oxides on the catalytic activity of these oxides is still ambiguous. Herein, typical metal oxides (ZnO/ZrO 2 ) with different crystal phases (monoclinic ( m -ZrO 2 ) and tetragonal ( t -ZrO 2 )) were employed for syngas conversion. The (ZnO/ m -ZrO 2 +SAPO-34) composite catalyst exhibited 80.5% selectivity for C 2 –C 4 olefins at a CO conversion of 27.9%, where the results are superior to those (CO conversion of 16.4% and C 2 –C 4 olefin selectivity of 76.1%) obtained over (ZnO/ t -ZrO 2 +SAPO-34). The distinct differences are ascribed to the larger number of hydroxyl groups, Lewis acid sites, and oxygen defects in ZnO/ m -ZrO 2 compared to ZnO/ t -ZrO 2 . These features result in the formation of more formate and methoxy intermediate species on the ZnO/ m -ZrO 2 oxides during syngas conversion, followed by the formation of more light olefins over SAPO-34. The present findings provide useful information for the design of highly efficient ZrO 2 -based catalysts for syngas conversion.
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高影响因子
Chemical Engineering and Processing-Process Intensification
·
2021
·
IF 4.237
Dicka Ar Rahim,Wei Fang,Gaojun Zhu,Haryo Wibowo,Dwi Hantoko,Qing Hu,Herri Susanto,Zengliang Gao,Mi Yan
Before syngas from gasification of biomass could be used as synthesis fuel or chemical feedstock, it requires the removal of hydrogen sulfide (H 2 S) to meet the purity standard level of those applications. In this study, Zn-Fe/Al 2 O 3 were successfully synthesized by a microwave-assisted wet incipient impregnation technique for use as adsorbent for H 2 S removal. The characterization of synthesized adsorbents showed that the oxide form of Zn and Fe present on the surface of adsorbents were zinc oxide (ZnO), magnetite (Fe 3 O 4 ), and zinc ferrite (ZnFe 2 O 4 ). While the reduction of adsorbent was mostly due to that of iron oxide . The reduced adsorbents might consist of ZnO/Fe 3 O 4 /FeO/Fe on alumina as support. At relatively high space velocity (26,000 h −1 ) the adsorbents were able to reduce the H 2 S concentration from 250 ppm at the inlet to around 45 ppm, 35 ppm, and 25 ppm at the outlet by adsorbent 1ZnFe, 2ZnFe, and 3ZnFe; respectively. The removal efficiency for adsorbent 1ZnFe, 2ZnFe, and 3ZnFe were 82%, 86%, and 90%; respectively. Results also shown an increase in adsorbent lifetime with the increase of the Zn to Fe ratio.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 27
·11808-11816
·
IF 3.288
Shi-Yuan Zhang,Jing-Jing Ma,Hong-Lin Zhu,Yue-Qing Zheng
Syngas, as a necessary feedstock dependent on non-renewable fossil fuels, is a mixture of CO and H2, which could be prepared by a renewable strategy via electrochemical CO2 reduction in water electrolyte solutions. Herein, beaded Au@Co3O4 nanowire arrays (denoted as Au@Co3O4 NAs) were obtained by immersion in HAuCl4 solution with Co3O4 nanowire arrays. The Au@Co3O4 NAs exhibited outstanding electrochemical performance of producing syngas via tuning from 1 : 1 to 4 : 1 with controlling voltage. In addition, the Au@Co3O4 NAs showed better catalytic performance for the oxygen evolution reaction with an overpotential of 320 mV at a current density of 50 mA cm−2, along with a small Tafel slope of 75 mV dec−1 in 1 M KOH solution. The electrochemical performance of Au@Co3O4 NAs is obviously superior to Co3O4 NAs, which will open up a viable strategy for the design and fabrication of a bi-functional electrocatalyst for the overall reaction (CO2 + H2O → CO + H2 + O2).
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高影响因子
RSC Advances
·
2015
·Vol. 5
·期 72
·58804-58812
·
IF 3.84
Ang Cao,Guilong Liu,Yizhi Yue,Lihong Zhang,Yuan Liu
A series of layered double hydroxides (LDHs) with different Cu/Co ratios were prepared according to the co-precipitation method and used as catalyst precursors for higher alcohol synthesis. The prepared samples were characterized by XRD, TPR, SEM, TEM and BET techniques. After calcination, the LDHs were transformed into a mixture of CuO, Co3O4, CuCo2O4 and alumina, and these oxides were mixed uniformly with sizes of several nanometers. For the sample with a ratio of Cu/Co = 1/2, the copper and cobalt species are mainly in the CuCo2O4 phase. In the reduction process, the superior mixed copper and cobalt species in nanoscale were reduced to Cu–Co alloy, which was confirmed by the XRD and TEM results. The prepared bimetallic catalysts showed high activity, good stability and very high selectivity to C2+ alcohols. With the best catalyst, CO conversion of 51.8%, selectivity to alcohols of 45.8% and 94.3 wt% of C2+OH in the total alcohols were obtained at 250 °C, 3 MPa and GHSV of 3900 mL (gcat h)−1.
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高影响因子
Molecular Catalysis
·
2024
·
IF 3.9
Jingjing Zhang,Yang Feng,Lixia Ling,Caiping Ma,Jungang Wang,Riguang Zhang,Maohong Fan,Bo Hou,Debao Li,Baojun Wang
The direct conversion of syngas to ethanol faces challenges due to catalyst inefficiencies and low ethanol yield. Bulk alloys with an appropriate atomic ratio can exhibit excellent catalytic performance. In this work, a series of Rh x Ni y (111) with different Rh/Ni ratios was rationally designed, and the ethanol preparation from syngas was explored based on density functional theory (DFT) calculation and microkinetic analysis. The results show that Rh 1 Ni 1 (111) was screened out to show optimum catalytic performance for ethanol production. This was attributed to a moderate quantity of charge transfer from Ni to Rh atoms, and a medium distance from the d -band center to the Fermi level. Further, to verify the catalytic performance of the catalysts at a Rh: Ni ratio of 1: 1, 1Rh1Ni/γ-Al 2 O 3 catalyst was prepared and its catalytic performance for ethanol preparation from syngas was investigated by comparing it with that of Rh/γ-Al 2 O 3 and Ni/γ-Al 2 O 3 . The catalytic performance of 1Rh1Ni/γ-Al 2 O 3 has been further confirmed to be preferred over Rh/γ-Al 2 O 3 and Ni/γ-Al 2 O 3 , achieving a 23.0 % CO conversion rate with 31.2 % ethanol selectivity.
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高影响因子
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