JOURNAL OF THE ENERGY INSTITUTE
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2024
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IF 5.6
Yanfang Zhu,Xu Jiang,Xiaoyuan Jin,Wenqi Song,Yuzhen Zhao
The catalytic properties of metals and metal oxides are vital for lignin depolymerization into phenolic and cyclohexane compounds production. This study investigated the lignin depolymerization of with different Ni content LaCoO 3 perovskite catalysts at different reaction conditions such as reaction temperature, time, catalysts amount. Furthermore, various hydrogen sources, including formic acid, ethanol, and pure hydrogen were tested. The highest bio-oil yield (75.3 wt%) was achieved with hydrogen under ethanol solvent, but selectivity for cyclohexane and phenolic monomers compound was low. Using formic acid (FA) with 7 % Ni-LaCoO 3 catalysts at 280 °C, a bio-oil yield of 72.4 wt% was obtained, with higher selectivity for 2,6-dimethoxyphenol (19.5 %), cyclohexane (18.5 %), and methylcyclohexane (14.2 %). This suggests that Ni with presence of FA facilitates the cleavage of lignin's β-O (C-O) and β-β (C-C) bonds efficiently. The reaction using FA, resulted in the lowest O/C ratio (0.06), highest H/C ratio (0.14), and the highest HHV (36.6 MJ/kg). The catalyst exhibited the highest reaction rate and hydrogenation activity, attributed to the presence of highly dispersed surface Co and Ni species. Notably, after three recycling test, the Ni-LaCoO 3 catalyst maintained very good catalytic activity. These results suggest that catalysts with this composite support have the potential to convert lignin-derived phenolic compounds into higher-grade hydrocarbon liquid fuels.
研究领域:
能源化学
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催化材料科学
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Zhenye Zhang,Shenghan Zhang,Shijie Wang,Xinliang Guo,Zhilin Wang,Yu Tan,KeXin Liang
Liquid organic hydrogen carriers (LOHCs) are considered highly promising materials for hydrogen storage due to their potential to store hydrogen under mild conditions. However, traditional hydrogenation and dehydrogenation methods for LOHCs often require harsh conditions and rely on exogenous hydrogen donors, limiting their practical application. Therefore, developing an efficient method to catalyze LOHCs hydrogenation and dehydrogenation at room temperature using a safe and clean hydrogen source is of significant scientific and practical importance. This paper presents an efficient and reversible electrochemical hydrogen storage system based on the nitrogen heterocyclic organic hydrogen carrier, quinoline. Here, the RuNi/NF electrode serves as an electrocatalyst to produce 1,2,3,4-tetrahydroquinoline (THQ) under ambient conditions, utilizing H 2 O as a hydrogen source with up to 99% conversion and 99% selectivity. Quinoline was synthesized with 94% conversion and 92% selectivity within the same solution system. This exceptional performance is attributed to the RuNi alloying effect, which enhances both the affinity of the active hydrogen atom (H∗) in the solution and the activity of Ni 2+ in the catalyst. Furthermore, the RuNi electrocatalyst exhibits excellent catalytic stability. The use of water as a hydrogen source eliminates the need for exogenous hydrogen, ensuring the safety of the process. This study provides an environmentally friendly and safe strategy for hydrogen storage in nitrogen heterocyclic organic carriers. By achieving efficient hydrogenation and dehydrogenation of LOHCs through electrochemical methods, this work not only expands the technical pathways for hydrogen storage but also offers important theoretical and practical insights for the development of future clean energy technologies.
研究领域:
能源科学
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催化化学
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产品关联
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2021
·Vol. 8
·期 21
·4712-4719
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IF 6.569
Tianxing Wu,Hanqi Meng,Rui Dang
Electrocatalytic hydrogenation is a competing reaction for hydrogen evolution that occurs in the presence of organic compounds containing unsaturated chemical bonds using water as the hydrogen donor. Here, we propose a simple method to synthesize amorphous Ta2O5 loaded amorphous Ru with poor crystallinity. The amorphous composite (Ta2O5/Ru-4.0-400) with an ultra-low Ru loading amount (2.16 wt%) exhibits 69.8% conversion of cinnamaldehyde with 29.1% FE and 100% selective formation of half-hydrogenated hydrocinnamaldehyde under a constant potential of −1.1 V vs. RHE for 5 h. Detailed experimental studies revealed that the amorphous structure with poor crystallinity offers structural flexibility and rich defects for electrochemical hydrogenation reactions, and the Ta2O5 substrate serves as a bridge to effectively facilitate electron transfer from Ru to CAL molecules. This work presents a new strategy for designing highly efficient electrocatalysts with an amorphous structure for the hydrogenation of organic compounds containing unsaturated chemical bonds.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
FUEL
·
2020
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IF 5.578
Jing-Pei Cao,Tao Xie,Xiao-Yan Zhao,Chen Zhu,Wei Jiang,Ming Zhao,Yun-Peng Zhao,Xian-Yong Wei
Selective hydrogenolysis, the aromatic ether C-O bonds under mild conditions, is crucial for the valorization of lignin. In this context, the effects of H 2 and solvent on the hydrogenolysis of lignin model compounds over Ru catalysts were explored. With H 2 as hydrogen donor, the Ru/AC exhibited the highest activity for converting lignin model compounds into monomeric compounds, whereas H 2 led to low selectivity of aromatics. However, isopropanol was the good H-donor solvent, which could provide a large amount of active hydrogen to promote the cleavage of C-O bonds. Additionally, the yield of aromatics in isopropanol was higher than that under H 2 atmosphere. It could be ascribed to the fact that isopropanol is the protic solvent which displays Lewis basicity, and is a good H-bond donor and a good H-bond acceptor. The higher electron-releasing inductive effect of isopropanol made it easier to provide active hydrogen. Based on the experiments, the mechanism of benzyl phenyl ether hydrogenolysis in H 2 and isopropanol system was presented.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
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2023
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IF 7.5
Fa-Peng Wu,Le-Le Qiu,Yun-Peng Zhao,Zong-Pin Fu,Jian Xiao,Jian Li,Fang-Jing Liu,Jing Liang,Jing-Pei Cao
Catalytic hydrodeoxygenation (HDO) of phenolic compounds is a promising strategy for bio-oil upgradation to produce high-value chemicals and fuels. Herein, a series of NiFeAlO x catalysts prepared by a co-precipitation method were applied in HDO of guaiacol as a typical model compound. The characterization results revealed that the catalyst with Ni/Fe/Al ratio of 3/0.5/2.5 possessed developed textural properties, small metal particles, abundant oxygen vacancies and acid sites. HDO of guaiacol occurred in two pathways with different hydrogen sources : the direct hydrogenation of benzene ring to 2-methoxycyclohexanone and the further hydrogenolysis and dehydration of intermediates to cyclohexane at 260 °C in n -hexane under H 2 for 6 h, while demethoxylation affording phenol followed by hydrogenation of phenol to cyclohexanol at 220 °C in isopropanol under N 2 for 2 h. The different product composition results from the type of reactive H species, where active hydrogen species are hydrogen radicals using H 2 as the hydrogen source and hydrogen ions with opposite charges using isopropanol as the H-donor solvent, respectively. The Ni 3 Fe 0.5 Al 2.5 O x catalyst maintained good performance after five recycle experiments with a slight decrease in the conversion of guaiacol. Moreover, the catalyst showed excellent universality for selective HDO of other phenolic compounds to cycloalkanes or cycloalkanols.
研究领域:
催化化学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Menghui Wei,Junchao Han,Qikang Wu,Jingjing Li,Zili Ji,Zhi Li,Jia Liang,Yanhui Guo
High water-source adaptability is meaningful to the popularization of hydrolysis of borohydrides as portable hydrogen generation technique. Herein, the key catalyst that can enable high water-sources adaptive hydrolysis of borohydrides is successfully developed for the first time. The as-prepared monolithic CoMoB based catalyst has outstanding catalytic activity with high hydrogen generation rate of the 3.0 L min −1 g −1 at 25 °C and low activation energy of 38.7 kJ mol −1 toward the hydrolysis of NaBH 4 using deionized water. More importantly, the catalyst exhibits distinguished durability toward hydrolysis of borohydrides in various water, including deionized water, lake water, and even seawater benefiting from its unique structure and gas scouring effect. Furthermore, an efficient NaBH 4 -based H 2 supply system is developed with the catalyst and this system successfully achieves full drive of 100 W fuel cell using different sources of water. This study may provide a new protocol to develop portable H 2 generation system with high water source adaptability in wild environments.
研究领域:
材料科学
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催化化学
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能源技术
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Yu Liu,Shiyue Bi,Zhanxin Song,Ziyi Song,Chao Xu,Mo Xian,Miaomiao Jin
Metal–enzyme cascade catalysis effectively combines the broad reactivity of chemical catalysis with the high selectivity of biocatalysis, improving reaction efficiency and simplifying the process flow through multiple sequential reactions in the same system. The introduction of exogenous palladium nanoparticles (Pd NPs) into Escherichia coli (E. coli) cells can significantly broaden the range of catalytic reactions facilitated by biological enzymes. Additionally, the targeted cytoplasmic synthesis of Pd NPs enhances their utilization efficiency in intracellular catalytic reactions while also eliminating the need for separating and purifying metals and enzymes. However, current methods largely enable the intracellular synthesis of Pd NPs in the periplasmic space and outer membrane. Moreover, the hydrogen sources commonly used in these methods─such as hydrogen (H2) and sodium borohydride (NaBH4)─carry safety risks. In this study, the mechanism of targeted synthesis of Pd NPs on the cytoplasmic side and its process were deeply investigated using a mild hydrogen source, sodium formate, in combination with genetic engineering and preparation conditions. And the constructed functional cell (Pd@E. coli) could catalyze benzaldehyde hydrogenation, with a conversion rate of 41.41% and benzyl alcohol yield of 17.68%, demonstrating considerable catalytic and loading stability. This study provides a reference for constructing catalytic systems for intracellular metal–enzyme cascades. Thus, it could bolster the development opportunities in the areas of non-natural products and drug development and provide ideas for addressing the drawbacks of existing biosynthetic technologies.
研究领域:
生物化学
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纳米生物学
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催化工程
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产品关联
DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2022
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IF 5.876
Kelong Ding,Ze-Nan Hu,Wenhui Zhang,Jiaxing Liang,Yiming Wang,Hong Li,Zejun Sun,Qionglin Liang,Hong-bin Sun
Chemoselective hydrogenation of nitrostyrene to aminostyrene still faces the trouble of low selectivity and poor activity. The bimetallic catalysts, which adjust the activity of noble metal nanoparticles through the doping of non-noble metals, are promising for selectively catalytic transfer hydrogenation (CTH). For another aspect, the hydrogen source also plays a vital role in selective CTH. Based on this, we prepared activity-inhibited bimetallic RhIn/ZIF-8 catalyst to study the catalytic performance towards different hydrogen sources (N 2 H 4 ·H 2 O, NaBH 4 , NH 3 ·BH 3 and H 2 ) and to explore the natural selectivity of these hydrogen sources. We found that the hydrazine hydrate was the most selective H-donor for the nitro group, while the H 2 had the highest natural selectivity to olefins . The H 2 produced from hydrazine hydrate is responsible for the formation of completely reduced products. The potential reduction by the intermediate imine did not occur to C C double bonds, this indicates controlling the decomposition of N 2 H 4 will enhance the selectivity of nitroarenes. Based on this, the reaction system with the catalyst bimetallic RhIn/ZIF-8 and N 2 H 4 ·H 2 O as the hydrogen source is established, which can fully reduce many nitrostyrenes with >98% selectivity to corresponding aminostyrenes.
研究领域:
催化化学
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材料科学
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有机合成
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2016
·Vol. 4
·期 41
·15920-15928
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IF 8.262
Lihua Li,Zhaoyong Lin,Lili Yu,Weijia Li,Guowei Yang
Water finding, collection and retention are important issues in drylands because of the rareness and high evaporation of water. Efficiently and fully utilizing water for photocatalytic hydrogen production is thus a challenge in desert areas. Inspired by the decent water absorption and retention properties of super absorbent polymers (SAPs), it is a bracing idea to use SAPs for water storage and hydrogen production reactors to enable full use of precious water for light-driven water splitting. Herein, for the first time, we have prepared a self-assembling solid-state hydrogen source (SHS) for photocatalytic hydrogen evolution. In the SHS, Pt/TiO2 and NiB/CdS nanocomposites were used as solar-driven and visible-light driven hydrogen production model catalysts, respectively, integrated with commercial agricultural acrylamide-acrylate copolymerized crosslinked SAP (AAC). It exhibits hydrogen production comparable to that of a typical suspension system, is reusable, and can be more readily recycled than conventional powdery catalysts, because of its monolithic structure. All water molecules in the SHS can be used to produce hydrogen. Accordingly, the SHS developed in this work offers a strategy for integrating SAPs with catalysts that would be practical in water-efficient photocatalytic hydrogen evolution in drought regions.
研究领域:
材料科学
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环境科学
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能源科学
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产品关联
DOI
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-10
·
IF 16.6
Yan Yong-Qing,Chen Ya,Wang Zhao,Chen Li-Hua,Tang Hao-Lin,Su Bao-Lian
Alkene feedstocks are used to produce polymers with a market expected to reach 128.4 million metric tons by 2027. Butadiene is one of the impurities poisoning alkene polymerization catalysts and is usually removed by thermocatalytic selective hydrogenation. Excessive use of H 2 , poor alkene selectivity and high operating temperature (e.g. up to 350 °C) remain the most significant drawbacks of the thermocatalytic process, calling for innovative alternatives. Here we report a room-temperature (25~30 °C) electrochemistry-assisted selective hydrogenation process in a gas-fed fixed bed reactor, using water as the hydrogen source. Using a palladium membrane as the catalyst, this process offers a robust catalytic performance for selective butadiene hydrogenation, with alkene selectivity staying around 92% at a butadiene conversion above 97% for over 360 h of time on stream. The overall energy consumption of this process is 0.003 Wh/mL butadiene , which is thousands of times lower than that of the thermocatalytic route. This study proposes an alternative electrochemical technology for industrial hydrogenation without the need for elevated temperature and hydrogen gas.
研究领域:
化学工程
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电化学
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催化
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
·
IF 20.2
Xiao-Shi Yuan,Sheng-Hua Zhou,San-Mei Wang,Wenbo Wei,Xiaofang Li,Xin-Tao Wu,Qi-Long Zhu
Electrocatalytic selective hydrogenation of α,β-unsaturated aldehydes represents a sustainable approach to achieve the highly value-added products, while the kinetic and selectivity are still greatly depend on the elaborated nanostructure design of electrocatalysts. In this study, by the sulfidation of ordered macroporous ZIF-67 single crystals, the ordered macroporous superstructure of carbon with abundant edge defects was achieved, where the tiny CoS nanoparticles are favorably anchored with homogeneous dispersion. Impressively, this superstructured electrocatalyst exhibited a remarkable activity towards the selective hydrogenation of cinnamaldehyde to hydrocinnamaldehyde with water as hydrogen source, acquiring the highest selectivity up to 92.1 % at 12 mA cm –2 with a cinnamaldehyde conversion of 89.6 %. The further experimental analysis combined with the density functional theory calculations revealed that the preferential absorption of C C over the tiny CoS nanoparticles with the maximal site accessibility, and the facilitated mass and charge transfer enabled by the ordered macropore engineering, jointly contribute to the excellent electrocatalytic performance. Additionally, this electrocatalyst also exhibited good expandability for several kinds of α,β-unsaturated aldehydes/ketones with different functional groups. Our findings offer new insights into the electrocatalytic selective hydrogenation, emphasizing the role of ordered pore engineering in constructing favorable microenvironments and synergizing active sites.
研究领域:
材料科学
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电化学
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催化
·
化工
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2024
·
IF 10.7
Jiaqi Chen,Wenbo Gao,Liangzhu Zhu,Haoliang Tao,Sheng Feng,Hujun Cao,Jianping Guo,Yanxia Chen,Ping Chen
Electrochemical ammonia synthesis (EAS) has emerged as a promising alternative to the traditional Haber–Bosch process. Indeed, N2 activation in room-temperature EAS systems remains a formidable challenge due to the strong NN bond. Solid oxide proton conductor EAS (PCEAS) electrolysis cells operating at intermediate temperatures offer a promising solution by utilizing both temperature and potential. In this process, the design of the cathode is crucial, requiring abundant proton and electron conduction channels, along with highly active catalysts. Herein, we design a cathode composed of ruthenium–La0.6Sr0.4Co0.2Fe0.8O3−δ–BaZr0.1Ce0.7Y0.1Yb0.1O3−δ (Ru–LSCF–BZCYYb) to meet the aforementioned requirements for PCEAS. LSCF and BZCYYb form a porous skeleton at the cathode, with Ru nanoparticles dispersed on the surface of this structure. This configuration features numerous triple-phase boundaries (TPBs), facilitating the contact between activated N2, H+, and e−, thereby promoting electrochemical ammonia synthesis. The impregnated Ru–LSCF–BZCYYb|BZCYYb|Ni–BZCYYb PCEAS electrolysis cell exhibited a maximum NH3 formation rate of 5.14 × 10−11 mol s−1 cm−2 and a maximum Faraday efficiency (FE) of 0.128% at 400 °C and −0.2 V with H2 and N2 as feedstock gases. Its yield surpassed those of the mixed Ru–LSCF–BZCYYb|BZCYYb|Ni–BZCYYb and the impregnated Ru–BZCYYb|BZCYYb|Ni–BZCYYb by a factor of 3.9 and 11.5, respectively. The authenticity of ammonia synthesis is confirmed using the 15N2 isotope combined with NMR detection. This study also achieved EAS using water as the hydrogen source. This approach would better meet the future demand for EAS by directly using N2 and H2O.
研究领域:
化学
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材料科学
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电化学
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催化
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）