INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2017
·
IF 2.843
Qilei Yang,Ang Cao,Na Kang,Hongyan Ning,Jiaming Wang,Zhao-Tie Liu,Yuan Liu
The catalytic performance of Cu–Co/Al2O3 in the slurry reactor for direct ethanol synthesis from syngas was investigated. The reduced catalyst and catalyst reacted for 100, 300, 500, and 750 h were characterized by using XRD, TEM, EDS, BET, and ICP-MS techniques. Compared with that in the fixed-bed reactor, the catalyst in the slurry reactor exhibited higher selectivity to ethanol, which was above 70 wt % in the total alcohols. The structure variation of the bimetallic Cu–Co with reaction time is that CuCo2O4 was transformed into Cu–Co alloy after reduction, and Cu–Co alloy was decomposed into Cu and Co after reaction for 100 h. After reaction for 300 h, Co2C started to generate and Cu@Co@Co2C was formed as reacted for 500 h. All of Cu–Co alloy, Cu@Co, and Cu@Co@Co2C are highly selective to ethanol, which was maintained for 750 h. Meanwhile, the slurry solvent of PEG-400 is another reason for the high ethanol selectivity.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Yuanjie Xu,Rong Chen,Hongqiao Lin,Qian Lv,Bo Liu,Lizhi Wu,Li Tan,Yihu Dai,Xupeng Zong,Yu Tang
Catalyst interface determines the activity and stability of partial oxidation of methane (POM) toward syngas under high temperatures crucially. Herein, Ni catalysts supported on CeO 2 were prepared under different pretreatment atmospheres to construct an optimal and robust interface. Ni/CeO 2 catalyst pretreated in H 2 (Ni/CeO 2 -H 2 ) exhibits the higher activity and the better stability than Ni/CeO 2 -Ar and Ni/CeO 2 -air catalysts. The Ni-O-Ce interfacial site in Ni/CeO 2 -H 2 catalyst shows the lower reduction temperature, indicating the enhanced H-spillover effect and enhanced oxidation resistance of Ni under POM conditions. Moreover, the XPS and in situ Raman results show that Ni/CeO 2 -H 2 contains more surface oxygen vacancies for adsorbing and activating oxygen, further contributing to the reaction activity. The in situ DRIFTS results indicate that the CH 4 could react with the lattice oxygen to form formate and carbonate, and further decompose to CO and CO 2 . These findings deepen the fundamental understanding of Ni/CeO 2 catalysts for POM reaction.
✓ 已验证
产品关联
DOI
高影响因子
Frontiers of Chemical Science and Engineering
·
2021
·Vol. 16
·期 4
·498-510
·
IF 4.204
Bo Jinxiao,Li Mei,Zhu Xinli,Ge Qingfeng,Han Jinyu,Wang Hua
The electrochemical conversion of CO 2 -H 2 O into CO-H 2 using renewable energy is a promising technique for clean syngas production. Low-cost electrocatalysts to produce tunable syngas with a potential-independent CO/H 2 ratio are highly desired. Herein, a series of N -doped carbon nanotubes encapsulating binary alloy nanoparticles (M x Ni-NCNT, M= Fe, Co) were successfully fabricated through the co-pyrolysis of mela-mine and metal precursors. The M x Ni-NCNT samples exhibited bamboo-like nanotubular structures with a large specific surface area and high degree of graphitization. Their electrocatalytic performance for syngas production can be tuned by changing the alloy compositions and modifying the electronic structure of the carbon nanotube through the encapsulated metal nanoparticles. Consequently, syngas with a wide range of CO/H 2 ratios, from 0.5:1 to 3.4:1, can be produced on M x Ni-NCNT. More importantly, stable CO/H 2 ratios of 2:1 and 1.5:1, corresponding to the ratio to produce biofuels by syngas fermentation, could be realized on Co 1 Ni-NCNT and Co 2 Ni-NCNT, respectively, over a potential window of −0.8 to −1.2 V versus the reversible hydrogen electrode. Our work provides an approach to develop low-cost and potential-independent electrocatalysts to effectively produce syngas with an adjustable CO/H 2 ratio from electrochemical CO 2 reduction.
研究领域:
材料科学
·
电化学
·
可再生能源
·
催化
✓ 已验证
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Junhao Lin,Jiaman Sun,Yi Chen,Juan Luo,Chongwei Cui,Shichang Sun
To directionally convert sludge into the high-quality syngas, the effects of various parameters on the biogas produced by the sludge microwave pyrolysis are explored, and the syngas generation mechanism under the synergistic effect of parameters is revealed. The results showed that the pyrolysis final temperature, reaction time, and the amount of the microwave absorber were the key factors that affected the biogas yield. A response surface analysis was used to explore the synergistic effect of each key parameter on the yield and the lower heating vale (LHV) of syngas. The pyrolysis temperature was the key to driving syngas generation. Properly prolonging the reaction time decreased the formation of tar by-products and increased the syngas yield. The addition of a microwave absorber increased the heating rate by enhancing the conversion efficiency of microwave energy, and this contributed to accelerating the dehydrogenation and the Boudouard reactions to promote the generation of H 2 and CO. Under high temperature conditions (900 °C), a higher syngas yield (10.25–34.31 mol/kg DS ) and LHV (4.85–14.53 MJ/kg DS ) were obtained in a shorter period time by synergistically optimizing the amount of microwave absorbers (8–10 g) and the reaction time (28–40 min). As the pyrolysis temperature increased, the H 2 content gradually rose to the peak, while the content of CO continued to increase. By analyzing the evolution of the specific pyrolysis products, the secondary pyrolysis of bio-oil at high temperatures and the Boudouard reaction were found to be the primary pathways that promoted syngas generation. This research provides strategic guidance for producing high-quality syngas using the microwave pyrolysis of waste biomass, thereby minimizing the exploration cost of basic experiments and providing directional control of the syngas quality.
研究领域:
环境科学
·
能源工程
✓ 已验证
DOI
高影响因子
BIORESOURCE TECHNOLOGY
·
2026
·
IF 8.2
Youn-Jun Lee,Chohee Yang,Deok Hyun Moon,Eilhann E. Kwon
CO 2 thermochemical treatment yielded MnO x -biochar and CO-rich syngas. • Micro- and mesopore development enhanced BPA adsorption by MnCCB (CO 2 ). • MnO x rich in Mn(IV) and Mn(III) promoted catalytic BPA oxidation. • Char gasification and oxygenate conversion increased yields of CO and H 2 . Adsorptive removal of aqueous organic pollutants is often limited by mass-transfer kinetics to the adsorbent surface. To address this constraint, integrated adsorption-oxidation processes have been widely explored as a strategic measure because they enable in situ degradation of adsorbent-bound organic pollutants, thereby regenerating active sites and prolonging removal performance. However, many such systems require energy inputs and chemical oxidants, which hinder practical implementation. Here, we evaluate MnO x -loaded corncob (CC) biochar produced under a CO 2 atmosphere (MnCCB (CO 2 )) as a bifunctional adsorption-oxidation material for bisphenol A (BPA) removal. Physicochemical characterization showed that CO 2 -assisted fabrication yielded MnO x with a higher oxidation state in MnCCB (CO 2 ) than that in the N 2 -derived analogue (MnCCB (N 2 )). MnCCB (CO 2 ) exhibited increased micro-/mesopore volume and a higher specific surface area. Consistent with these structural advantages, MnCCB (CO 2 ) achieved a BPA removal rate constant of 8.48 × 10 -2 min −1 , outperforming MnCCB (N 2 ) and pristine CC biochars produced under either N 2 or CO 2 . Beyond pollutant removal, Mn-catalyzed CO 2 mediated thermochemical treatment also enhanced syngas formation during MnCCB (CO 2 ) production. This improvement is attributed to selective catalytic reactions between bio-oil and CO 2 , during which CO 2 is converted to CO in the presence of MnO x . Overall, this work demonstrates the potential of CO 2 -assisted thermochemical treatment for the simultaneous production of functional biochar and syngas. Download: Download high-res image (121KB) Download: Download full-size image
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·123788
·
IF 7.5
Mingtao Hu,Huiwen Wu,Wenyi Deng,Lingyu Tai,Xuerong Zheng,Weihao Li,Yaxin Su,Run Xu
Catalytic tar reforming is a pivotal technology for upgrading syngas quality during sewage sludge gasification. In this study, a series of Ni-modified carbon-based catalysts (x%NiFe/C) were synthesized using MIL-100(Fe) as a precursor to investigate the impact of Ni-loading on the catalytic performance for tar reforming. Detailed characterizations, including XRD, XPS, Raman, and NH 3 -TPD, revealed that the introduction of Ni species significantly tailored the physicochemical properties of the catalysts. Specifically, the 3.3%NiFe/C catalyst exhibited the optimal specific surface area and pore structure, facilitating efficient mass transfer. Characterization results confirmed the formation of Ni-Fe alloy, which not only modulated the surface electronic density to optimize acidity but also enhanced the dispersion of active sites. The interaction between Ni and Fe species effectively promoted the cleavage of C-C and C-H bonds in tar molecules while suppressing carbon deposition. Consequently, the 3.3%NiFe/C catalyst demonstrated superior catalytic activity and stability in the two-stage microwave-assisted gasification reforming process, achieving a syngas yield of 555 mg/g·SS, a tar conversion rate of 82.9%, and an H 2 concentration of 73.8 vol%. After ten cycles, the H 2 yield and concentration remained as high as 28.0 mmol/g·SS and 68.2 vol%, respectively. This work provides mechanistic insights into the design of MOF-derived carbon-supported catalysts for efficient SS gasification.
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
Zhi-Hao Wang,Jing-Pei Cao,Wen Tang,Zi-Meng He,Fei-Long Yang,Ze-Ying Wang,Xiao-Yan Zhao
Recovering beneficial metal ions from industrial effluents by suitable support can be an efficient and environment-friendly way to prepare specific catalysts directly. Herein, modified lignite was developed as an ion exchange material and used to prepare Co-Cu bimetallic catalysts for hydrogen-rich syngas production from steam reforming reactions. For all the catalysts studied, Co 75 Cu 15 /600 (carbonization temperature at 600 °C) exhibits the optimal catalytic activity and stability in both steam reforming of toluene and biomass tar under low temperatures. Fresh and spent catalysts were detailedly characterized to investigate the metal interactions and catalyst deactivation. The introduction of Cu contributes to the formation of Co-Cu alloy and the lower particle size of Co (4.17 nm), thereby suppressing the carbon deposition, the oxidation of metals and the change of catalyst structure after reaction. Therefore, the inexpensive and readily-available Co-Cu/C has the potential to serve as a promising catalyst for large-scale biomass gasification technology.
✓ 已验证
产品关联
DOI
高影响因子
ENERGY
·
2022
·
IF 8.857
Xiaopeng Shi,Pan Li,Xianhua Wang,Jiande Song,Shuqi Fang,Chun Chang,Shusheng Pang
The main purpose of this work was to explore the effect of metal modified biochar and multi-catalysts on improving the quality of products by microwave pyrolysis (MVP) of biomass. Single-component catalysts and multi-catalysts were prepared by Zn/Zr impregnation methods. The prepared catalysts were evaluated by XRD , BET, FT-IR and SEM. The properties, composition and product distribution of bio-oil and bio-syngas were analyzed. The results showed that ZSM-5 obtained more bio-oil (42.16 wt%) at the expense of gas product yield, and BC obtained the highest gas yield (43.10 wt%). Zn promoted the selectivity of aromatic hydrocarbons in bio-oil, Zr could effectively improve the yield of syngas and upgrading bio-oil, respectively. Zr-modified multi-catalyst was prepared, and the highest syngas yield (91.54 vol%) and aromatic hydrocarbon products were obtained. Among them, the selectivity of monocyclic aromatic hydrocarbons (MAHs) reached 21.82%. The mechanism of MVP of biomass under the effect of Zn/Zr modified different catalysts was proposed. The study has successfully demonstrated an approach for producing high-value bio-oil and bio-syngas from microwave multi-catalyst pyrolytic system.
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
·
IF 3.141
Shaoxia Guo,Shuangshuang Li,Huixian Zhong,Dandan Gong,Jiaming Wang,Na Kang,Lihong Zhang,Guilong Liu,Yuan Liu
A novel scheme is designed to prepare superior catalysts with good activity, high selectivity, outstanding stability, excellent resistance to sintering and carbon deposition. In the scheme, the ions of lanthanum, strontium, cobalt, and gallium were confined into La1–xSrxCo0.65Ga0.35O3 with perovskite structure and uniformly dispersed at the atomic level; by reducing La1–xSrxCo0.65Ga0.35O3, a strong interaction between the active sites and promoters exists, and good catalytic performance for direct ethanol synthesis (DES) can be obtained. According to the design scheme, a series of La1–xSrxCo0.65Ga0.35O3 (x = 0–0.4) and La0.7Sr0.3CoO3 (LSC) catalysts were prepared by citric acid complexation method and characterized by XRD, H2-TPD, TPR, TEM, BET, XPS, and TG techniques. Thanks to the excellent catalyst design scheme, the catalyst reduced from La0.7Sr0.3Co0.65Ga0.35O3 showed good activity, high selectivity, and excellent stability for DES. Simultaneously, this catalyst design scheme can be extended to the design of other catalysts.
研究领域:
催化化学
·
材料科学
·
化学工程
·
能源化学
·
纳米技术
✓ 已验证
DOI
高影响因子
WASTE MANAGEMENT
·
2021
·
IF 7.145
Junhao Lin,Shichang Sun,Juan Luo,Chongwei Cui,Rui Ma,Lin Fang,Xiangli Liu
This paper proposed to use ferric oxide (Fe 2 O 3 ) and ferroferric oxide (Fe 3 O 4 ) as catalysts with both microwave absorption and catalytic properties. Carbon dioxide (CO 2 ) was introduced as the reaction atmosphere to further improve the quality of biofuel produced by microwave pyrolysis of food waste (FW). The results showed the bio-gas yield and the syngas concentration (H 2 + CO) increased to 70.34 wt% and 61.50 mol%, respectively, using Fe 3 O 4 as the catalyst. The content of aliphatic hydrocarbons in bio-oil produced with the catalyst Fe 2 O 3 increased to 67.48% and the heating value reached 30.45 MJ/kg. Compared with Fe 2 O 3 catalyst, Fe 3 O 4 exhibited better microwave absorption properties and catalytic properties. Transmission electron microscopy (TEM) and Electron paramagnetic resonance (EPR) characterizations confirmed that the crystal surface of Fe 3 O 4 formed more oxygen vacancy defects and unpaired electrons. Additionally, according to the X-ray photoelectron spectroscopy (XPS) analysis, the content of lattice oxygen in Fe 3 O 4 was 14.11%, a value that was much lower than Fe 2 O 3 (38.54%). The oxygen vacancy defects not only improved the efficient utilization of microwave energy but also provided the reactive sites for the reaction between the volatile organic compounds (VOCs) and CO 2 to generate CO. This paper provides a new perspective for selecting catalysts that have both microwave absorption and catalytic properties during the microwave pyrolysis of biomass.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Xinyao Zou,Chao Ma,Ang Li,Zhan Gao,Zulipiya Shadike,Kun Jiang,Junliang Zhang,Zhen Huang,Lei Zhu
Electrochemical conversion of CO2 to the syngas hybrid with the Fischer–Tropsch (FT) process is a promising way to produce synthetic fuels from renewable energy sources. The product distribution in liquid hydrocarbons produced by FT synthesis has strong dependence on the CO/H2 ratio of the syngas feedstock. Herein, we demonstrated the feasibility of tuning the CO/H2 ratio at a wide range by developing nanoparticle-assisted Ni–Co binary single-atom catalysts for electrocatalytic production of syngas. By controlling the elemental proportion of Ni–Co in the composite catalysts, electrochemical reduction of CO2 to syngas with a tunable CO/H2 ratio from 0.3 to 27.6 was achieved. For the binary catalysts with a Ni–Co ratio of 1:1, the CO/H2 ratio maintains at 1.3–1.5 in a broad potential range from −0.59 to −0.83 V versus reversible hydrogen electrode (RHE) and the total current density reaches ∼32.2 mA/cm2 at −1.0 V versus RHE. The promotion effect of nanoparticles on Ni–Co single-atom catalysts was validated by partial removal of nanoparticles and further density functional theory (DFT) calculations. As revealed by DFT calculations, nanoparticles incorporated in single-atom sites take essential roles in facilitating the adsorption of CO2 and the formation of *COOH. The origin of CO2RR and hydrogen evolution reaction reactivities can be identified as Ni–N4 and Co–N4 single-atom sites, respectively. The dual active sites allow the facile control of the CO/H2 ratio of electrochemical converted syngas, and it will be beneficial to downstream production of diverse chemicals.
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Zhige Zhang,Guican Bi,Shenglong Zhang,Tao Tan,Jun Xie
The use of biogas as renewable raw material to produce syngas（H 2 /CO ≈ 2）suitable for direct synthesis of methanol has attracted wide attention, but designing promising catalysts with high activity and stability remains a challenge. The catalytic systems used for this process usually have the characteristics of poor stability and easy carbon deposition. Here, Based on the Ce redox cycle and the strong metal-support interaction (SMSI), we designed and synthesized a series of Ni catalysts (denoted as Ni/CeMgO x /BN) with BN interfacial constraints. The abundant oxygen vacancy of reaction-induced Ce redox cycle endows Ni/CeMgO x /BN with excellent carbon resistance, because the ability to activate CO 2 /H 2 O is significantly enhanced. The CO 2 /H 2 O activation and carbon elimination mechanism were comprehensively characterized by in situ H 2 -TPR/CO 2 /H 2 O-TPSR, in situ CH 4 -TPSR/CO 2 /H 2 O-TPO, and FTIR, etc. Ascribed to the appropriate basicity of CeMgO x , homogeneous Ni dispersion, and strong interaction between Ni ultra-small nano particles (NPs) and CeMgO x /BN, Ni/CeMgO x /BN exhibit higher CO 2 /H 2 O adsorption/activation, higher CH 4 activation/dissociation, compared with another samples, which facilitate the formation of active oxygen species and intermediate coke removal, thus enhance the resistance to coke deposition and sintering. At 750 °C, Ni/CeMgO x /BN exhibit satisfying catalytic activity (CH 4 /CO 2 conversation 92 %/52 %) and superior stability (100 h) with negligible deactivation rates.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）