Frontiers of Environmental Science & Engineering
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2022
·Vol. 17
·期 3
·1-12
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IF 6.048
Gao Yuchen,Jiang Jianguo,Meng Yuan,Ju Tongyao,Han Siyu
Biogas is a renewable biomass energy source mainly composed of CH 4 and CO 2 . Dry reforming is a promising technology for the high-value utilization of biogas. Some impurity gases in biogas can not be completely removed after pretreatment, which may affect the performance of dry reforming. In this study, the influence of typical impurities H 2 S and NH 3 on dry reforming was studied using Ni/MgO catalyst. The results showed that low concentration of H 2 S in biogas could cause serious deactivation of catalyst. Characterization results including EDS, XPS and TOF-SIMS confirmed the adsorption of sulfur on the catalyst surface, which was the cause of catalyst poisoning. We used air calcination method to regenerate the sulfur-poisoned catalysts and found that the regeneration temperature higher than 500 °C could help catalyst recover the original activity. NH 3 in the concentration range of 50–10000 ppm showed a slight inhibitory effect on biogas dry reforming. The decline rate of biogas conversion efficiency increased with the increase of NH 3 concentration. This was related to the reduction of oxygen activity on catalyst surface caused by NH 3 . The synergetic effect of H 2 S and NH 3 in biogas was investigated. The results showed that biogas conversion decreased faster under the coexistence of H 2 S and NH 3 than under the effect of H 2 S alone, so as the surface oxygen activity of catalyst. Air calcination regeneration could also recover the activity of the deactivated catalyst under the synergetic effect of H 2 S and NH 3 .
研究领域:
能源化学
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催化化学
✓ 已验证
DOI
高影响因子
AICHE JOURNAL
·
2014
·Vol. 60
·期 6
·2254-2262
·
IF 2.581
Jifeng Pang,Mingyuan Zheng,Aiqin Wang,Ruiyan Sun,Hua Wang,Yu Jiang,Tao Zhang
Miscanthus, a promising energy crop, was used for ethylene glycol (EG) production through one-pot catalytic conversion. With a binary catalyst composed of commercial tungstic acid and Raney Ni, the miscanthus with 1 % concentration was transformed into EG with a yield of 35.5%. However, the yield dropped to 13.6% as the miscanthus concentration was increased to 10 %. The underlying reason for the yield decrease was disclosed through analysis of the liquid products, investigation of pretreatments, and characterization of the catalysts. It was found that the protectors on the surface of miscanthus and the lignin component underwent decomposition under reaction conditions, resulting in the formation of some organic acids and unsaturated compounds that preferentially poisoned the Raney Ni catalyst and consequently decreased the EG yield. When the inhibitors were effectively removed by base solvent pretreatment, the EG yield was successfully improved to 39.0% even under 10% concentration of feedstock. © 2014 American Institute of Chemical Engineers AIChE J , 60: 2254–2262, 2014
研究领域:
生物能源
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催化化学
✓ 已验证
DOI
高影响因子
Catalysts
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2025
·Vol. 15
·期 6
·530
·
IF 4
Yalin Guo,Zhuang Ma,Binbin Jin,Limin Ma,Guodong Yao
The sustainable valorization of lignocellulosic biomass into high-value platform chemicals presents a crucial pathway for reducing reliance on fossil resources. Gamma (γ)-valerolactone (GVL) has gained recognition as a versatile bio-derived compound with broad applications in renewable energy systems and green chemical synthesis. While conventional GVL production strategies from carbohydrate biomass typically depend on noble metal catalysts paired with high-pressure hydrogen gas, these approaches face substantial technical barriers including catalyst costs, hydrogen storage requirements, and operational safety concerns in large-scale applications. This work develops an innovative catalytic system utilizing earth-abundant iron for in situ hydrogen generation through water splitting, integrated with Raney Ni as the hydrogenation catalyst. The designed two-stage process enables direct conversion of cellulose—first through acid hydrolysis to levulinic acid (LA) followed by catalytic hydrogenation to GVL without intermediate purification. Through systematic parameter optimization, a remarkable 61.9% overall GVL yield from cellulose feedstock was achieved. Furthermore, the methodology’s versatility was demonstrated through wheat straw conversion experiments, yielding 24.6% GVL. This integrated methodology explores a technically feasible pathway for direct cellulose-to-GVL conversion utilizing abundant water as the hydrogen source, effectively overcoming the critical limitations associated with conventional hydrogenation technologies regarding hydrogen infrastructure and process safety.
研究领域:
生物化学
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可再生能源
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS TODAY
·
2016
·
IF 4.312
Kun Jiang,Dong Sheng,Zihao Zhang,Jie Fu,Zhaoyin Hou,Xiuyang Lu
Mixed MgO–Al 2 O 3 (with different Mg/Al ratio) supported nickel catalysts were prepared via co-precipitation method and used for hydrogenation of levulinic acid to γ-valerolactone under mild condition. Characterization results indicated that mixed MgO–Al 2 O 3 supported Ni catalysts possessed bigger surface area than that of Ni/MgO and Ni/Al 2 O 3 , and Ni dispersed highly on the surface of mixed MgO–Al 2 O 3 support. It was found that mixed MgO–Al 2 O 3 supported Ni catalysts were more active and selective for the hydrogenation of levulinic acid to γ-valerolactone than that of Ni/MgO and Ni/Al 2 O 3 , and the best yield of γ-valerolactone at 160 °C, 1 h and 3 MPa H 2 reached 99.7% over Ni/MgAlO 2.5 , and Ni/Mg 2 Al 2 O 5 could be recycled without obvious loss of its initial activity.
研究领域:
化学工程
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 10
·4136
·
IF 4.6
Yongwang Ren,Huizhong Xu,Beibei Han,Jing Xu
At present, the selective hydrogenation of α, β-unsaturated aldehydes remains a challenge due to competition between unsaturated functional groups (C=C and C=O). In this study, N-doped carbon deposited on silica-supported nickel Mott–Schottky type catalysts (Ni/SiO2@NxC) was prepared for the selective hydrogenation of cinnamaldehyde (CAL) by using the respective hydrothermal method and high-temperature carbonization method. The prepared optimal Ni/SiO2@N7C catalyst achieved 98.9% conversion and 83.1% selectivity for 3-phenylpropionaldehyde (HCAL) in the selective hydrogenation reaction of CAL. By constructing the Mott–Schottky effect, the electron transfer from metallic Ni to N-doped carbon at their contact interface was promoted, and the electron transfer was demonstrated by XPS and UPS. Experimental results indicated that by modulating the electron density of metallic Ni, the catalytic hydrogenation of C=C bonds was preferentially performed to obtain higher HCAL selectivity. Meanwhile, this work also provides an effective way to design electronically adjustable type catalysts for more selective hydrogenation reactions.Keywords:Ni catalyst;N-doped carbon;electronic effect;cinnamaldehyde hydrogenation
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CATALYSIS TODAY
·
2024
·
IF 5.2
Yushuai Sang,Mingze Yang,Hong Chen,Yongdan Li
Catalytic lignin solvolysis (CLS) holds promise for efficient lignin utilization, yielding small molecules with minimal or no char formation. However, the role of different active sites of catalyst in CLS are rarely discussed. Here, Ni catalysts on different supports, i.e., SiO 2 , Al 2 O 3 , MgO, and ZrO 2 , were prepared with the aim of manipulating the relative importance of metal and acid-base functionalities to investigate the role of different active sites in the enzymatic hydrolysis of lignin (EHL) ethanolysis. The main ether linkage, i.e., β-O-4, in EHL is cleaved without the participation of a catalyst. Metal sites suppress repolymerization through hydrogenating active intermediates, while acid and base sites facilitate the conversion of phenolic monomers into complex alkylated and etherified products and also promote repolymerization reactions. Among the catalysts, Ni/SiO 2 demonstrated the highest hydrogenation activity and yielded the most monomers (24.7 wt %) at 280 °C for 6 h under 2 MPa H 2 in ethanol. These findings shed light on the catalytic mechanisms in CLS, offering valuable insights for future catalyst design.
研究领域:
化学工程
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催化科学
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生物质利用
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2013
·
IF 3.41
Qiying Liu,Hualiang Zuo,Tiejun Wang,Longlong Ma,Qi Zhang
Nano-sized SAPO-11s were hydrothermally synthesized with using di-n-propylamine (DPA) as structure-directing agent in mixed n-tetradecanoamine–n-propanol–H 2 O medium and the Ni/SAPO-11 catalysts were prepared by incipient wetness impregnation. The catalysts was characterized by XRD, SEM, BET, H 2 -TPR, NH 3 -TPD and TG techniques and their catalytic performance was tested in hydrodeoxygenation (HDO) of palm oil to hydrocarbon fuels. Surfactant n-tetradecanoamine could mediate the minimum SAPO-11 sizes into 20–50 nm. As comparing to the commercial SAPO-11, the nano-sized SAPO-11s presented significantly enlarged surfaces and mesoporous volumes, which offered sufficient space and strong interactions for dispersing Ni. One-step HDO of palm oil demonstrated that the nano-sized SAPO-1 supported Ni catalysts showed the high yield (80%) of liquid hydrocarbons, high isomerization selectivity (80%) and excellent stability due to that the catalyst presented appropriate acidity, higher Ni dispersity, balance of metal (Ni) and acid (SAPO-11) functionalities and fast diffusion for bulky palm oil and products. These promotion effects observed over the nano-sized SAPO-11 supported Ni catalysts indicated the potential application in biorefinery of vegetable oils to hydrocarbon fuels.
研究领域:
催化化学
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可再生资源转化
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能源材料科学
✓ 已验证
DOI
高影响因子
FUEL
·
2021
·
IF 6.609
Tao Pan,Sida Ge,Mengnan Yu,Yana Ju,Ran Zhang,Pei Wu,Kuanyu Zhou,Zhijie Wu
Zn modified ZSM-5 zeolite supported Ni bifunctional catalysts were prepared by in-situ hydrothermal synthesis (Zn-Ni-ZSM-5), co-impregnation method (Zn-Ni/ZSM-5) as well as combining in-situ hydrothermal synthesis of Zn-ZSM-5 and sequential impregnation of Ni (Ni/Zn-ZSM-5) and used for the selective converting olefin to aromatics applicable for FCC gasoline hydro-upgrading. The Lewis (L) acid sites generated by ZnOH + species and hydrogenation active sites from Ni 0 species were varied with preparation method, in which their locations at the external surface or micropores of zeolite changed the acid properties of catalysts. Comparing to the Zn-Ni/ZSM-5 from the co-impregnation method, direct in-situ hydrothermal method could incorporate Zn and Ni species within zeolite, which makes the strong interaction between the metal species and the framework Al to form medium-strong L acids (ZnOH + /NiOH + ). This leads to the decrease of ratio of Brønsted acid sites to L acid sites (B/L) from 0.40 to 0.12 and the difficulty in reducing of Ni cations to Ni 0 from 57% to 30% Ni 0 percent. Ni/Zn-ZSM-5 sample prepared by incorporating Zn species into micropores and sequential depositing Ni species at the external surface of zeolite possesses a low B/L ratio similar to Zn-Ni-ZSM-5 (0.20 versus 0.12) but a much higher Ni 0 percent (52% versus 30%). Zn-Ni-ZSM-5 shows closer intimacy between Zn and Ni species comparing to Zn-Ni/ZSM-5 and Ni/Zn-ZSM-5. For the 1-hexene aromatization, the formed iso -alkene at acid sites was quickly saturated to iso -alkanes by the adjacent Ni 0 particles over Ni-Zn-ZSM-5 catalyst in hydrogen steam. However, the location of aromatization active sites (ZnOH + , L acid sites) in micropores and hydrogenation active sites (Ni 0 species) on external surface of Ni/Zn-ZSM-5 makes the tandem conversion of n-alkene → iso -alkene → aromatics, rather than the n-alkene → iso -alkene → iso -alkane. Thus, Zn-Ni-ZSM-5 with close intimacy of ZnOH + and Ni 0 particles shows a high iso -alkane selectivity (27.9% iC 4 + ), while Ni/Zn-ZSM-5 exhibits a high aromatics selectivity (39.6 %) in the conversion of 1-hexene in hydrogen steam. Similar results have also found in the conversion of n-heptane. Here, the control of the intimacy of Zn and Ni in ZSM-5 zeolites has been realized to be a good protocol to adjust the selective conversion of olefins/alkanes to aromatics versus iso -alkanes.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Processes
·
2025
·Vol. 13
·期 4
·1110
·
IF 2.8
Shikang Zhao,Guohong Chen,Kaiqi Zheng,Shaojie Li,Jiaqi Xu,Fanan Wang,Xueping Liu,Rengui Weng
γ-Valerolactone (GVL) is a promising bio-based platform molecule with significant potential for energy applications. The production of GVL via biomass-based levulinic acid (LA) is an important reaction. To enhance the conversion and selectivity of non-precious-metal catalysts in the LA-to-GVL process and to better understand the key factors influencing this conversion, we conducted a series of experiments. In this study, supported Cu-Ni bimetallic catalysts (Cu-Ni2/Al2O3) were prepared using layered double hydroxides (LDHs) as a precursor. Compared with Cu-Ni catalysts synthesized via the conventional impregnation method, the Cu-Ni2/Al2O3catalysts exhibit higher catalytic activity and stability. The results demonstrated that efficient conversion was achieved with isopropanol as the hydrogen donor solvent, a reaction temperature of 180 °C, and a reaction time of 1 h. The yield of GVL reached nearly 90%, with a decrease of approximately only 6% after six consecutive cycles. The Cu-Ni2/Al2O3catalyst proved to be effective for converting biomass-derived LA to GVL, offering a route that not only reduces production costs and environmental impact but also enables efficient biomass-to-energy conversion.
研究领域:
催化化学
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能源科学
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生物质利用
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF RARE EARTHS
·
2022
·
IF 4.632
Tingting Bao,Hui zhou,Yi Zhang,Chenxu Guo,Wenming Guo,Hang Qin,Pengzhao Gao,Hanning Xiao,Weixiong Liu
Ni/CeO 2 catalysts ( n CeO2 : n Ni = 0, 1, 4, 7, 10) supported on SiC porous ceramics for ethanol steam reforming (ESR) were investigated with respect to hydrogen production performance and growth of carbon deposition. The oxygen released from CeO 2 enables the oxidation of CH x species to serve as carbon precursors, thus providing Ni/CeO 2 catalysts with stronger resistance to carbon deposition compared with Ni catalysts. The Ni/CeO 2 catalysts prepared by inverse microemulsion and impregnation methods exhibit regular semicircular spherical shape on SiC porous ceramics. Under 500 °C for 25 h of ESR reaction, the ethanol conversion rate over Ni/CeO 2 catalysts ( n CeO2 : n Ni = 7) is sustained up to 100% and H 2 selectivity is essentially kept at 74%. The by-product selectivity declines stepwise with increasing content of CeO 2 , which is attributed to the adsorption and oxidation of CO and of CH x species as CH 4 precursor from CeO 2 . The scanning electron microscopy (SEM) and transform electron microscopy (TEM) results reveal that further loading of CeO 2 on the surface of Ni catalysts can alleviate both migration and sintering of Ni particles. Furthermore, carbon deposition on Ni/CeO 2 catalysts preferentially outgrow filamentous rather than amorphous carbon , with a tendency for the latter to be more deactivated.
研究领域:
催化化学
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材料科学
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能源化学
✓ 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.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Jia-qi Bai,Mei Ma,Huangfei Liu,Zhangkai Qian,Durui Liu,Yuncai Zhao,Yijing Gao,Jingshuai Chen,Mengdie Cai,Song Sun
The hydrogenation of nitriles is an environmentally friendly and atom-economical route to prepare high-value amines; however, it is still a challenge to control selectivity because of the occurrence of hydrogenation, self-coupling, and hydrogenolysis reactions during the hydrogenation process. It is highly desirable to develop efficient non-noble-metal catalysts for the hydrogenation of nitriles to secondary amines, although several noble metal catalysts have been reported. Herein, we successfully prepared a Cu–Ni/W20O58 catalyst and found that the Cu4.4–Ni0.6/W20O58 catalyst showed a 92.3% yield with initial TOFs of 270.0 h–1 at 373 K and 3 MPa H2 for the hydrogenation of benzonitrile (BN) to dibenzylamine (DBA), which was much superior to that of the monometallic Cu4.4/W20O58 and Ni0.6/W20O58 catalysts. Moreover, the Cu4.4–Ni0.6/W20O58 catalyst could be reused at least 4 times and was effective for the hydrogenation of various nitriles with superior selectivity to secondary amines. Furthermore, the reaction mechanism of BN hydrogenation for the Cu–Ni alloy of Cu4.4–Ni0.6/W20O58 was proposed on the basis of spectroscopic studies such as XRD, TPR, TEM, XAFS, and XPS, kinetic studies such as the effect of BN concentration and H2 pressure, the isotopic effect of hydrogen, and the effect of the reaction temperature and DFT calculations. The rate-determining step was the hydrogenation of benzylidenamine (BI) to the half-hydrogenated intermediate by one H atom over the Cu4.4–Ni0.6/W20O58 catalyst. The Ni–W20O58 interface was responsible for the adsorption and activation of BN, and the electron-rich Cu acted as the site for H2 dissociation; the synergistic effect of Cu and Ni led to the superior catalytic performance of the Cu4.4–Ni0.6/W20O58 catalyst.
研究领域:
催化化学
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材料科学
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环境化学
✓ 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）