JOURNAL OF THE ENERGY INSTITUTE
·
2019
·
IF 3.774
Yun-Peng Zhao,Fa-Peng Wu,Qing-Lu Song,Xing Fan,Li-Jun Jin,Rui-Yu Wang,Jing-Pei Cao,Xian-Yong Wei
In this work, a bimetallic catalyst of Pd and Ni supported on HZSM-5 was designed and evaluated in the hydrodeoxygenation of model compounds representing various C–O bonds in lignin. The effects of temperature, holding time, and initial H 2 pressure on the catalytic performance of the Pd–Ni/HZSM-5 catalyst were investigated. The results indicated that the Pd–Ni/HZSM-5 catalyst exhibited superior catalytic activity towards the conversion of the model compounds to alkanes compared to its monometallic counterparts. Direct cleavage of the C–O bond in DPE was achieved under low H 2 pressure, mainly producing benzene and minor amounts of phenol and cyclohexane, while at high H 2 pressure, the reaction pathway was altered towards hydrogenation of the benzene ring , followed by then cleavage of the C–O bond to afford only cyclohexane. Moreover, the Pd–Ni/HZSM-5 catalyst showed high activities when applying other substrates including anisole, veratrole, guaiacol, benzyloxybenzene, phenethyl phenyl ether, and dibenzyl ether.
研究领域:
催化化学
·
能源化学
✓ 已验证
DOI
高影响因子
Cell Reports Physical Science
·
2024
·
IF 7.9
Qiang Wang,Ling-Ping Xiao,Qian Xu,Heng Zhang,Changzhi Li,Run-Cang Sun
Reductive catalytic fractionation of lignocellulose is a promising biorefinery strategy that combines biomass fractionation with lignin depolymerization. Herein, we report a layered copper silicate nanotube (RCuSNT) catalyst, which exhibits enhanced performance toward reductive fractionation of lignocellulose. The phenolic monomers obtained from lignin are close to the theoretical maximum yields (22.5 wt% for softwoods and 38.5 wt% for hardwoods), with high selectivity for propyl and propanol end-chain phenolic compounds. The result indicates that lignin is successfully deconstructed while cellulose and hemicellulose are retained essentially intact (88.4 wt%). The catalyst shows stability in recovery experiments, which is attributed to the immobilization of copper species by the leaf silicate. Moreover, a series of lignin model compounds and isotope-labeled reactions clarify the mechanism of C–O bond scission over RCuSNTs. This work provides a significant benchmark for the rational development of inexpensive metal catalysts in reductive catalytic fractionation systems for lignin valorization.
研究领域:
生物化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2020
·
IF 7.888
Jie Zhang,Chuang Li,Weixiang Guan,Xiaozhen Chen,Xiao Chen,Chi-Wing Tsang,Changhai Liang
Co(Ni)/MoO 3 catalysts were prepared, characterized and evaluated for the hydrogenolysis of bio-derived dibenzofuran (DBF), aiming at the understanding of the promoting effect of Co/Ni on MoO 3 for high-yield production of aromatic products. All Co(Ni)/MoO 3 catalysts selectively cleaved C-O bond, thus effectively transformed DBF to biphenyl (BP) at relatively moderate conditions. The experimental results from varying Mo species by adjusting the reduction temperature of MoO 3 together with XPS and in-situ XRD characteristic were evident that Mo 5+ species was responsible as the major active specie for the reaction. Promotional effect between Co(Ni) and Mo in Co(Ni)/MoO 3 catalysts was observed, resulted from the presence of acidic Co(Ni)MoO 4 species and a large number of Mo 5+ species both of which were created local to the Co(Ni)-O-Mo interface, as can be characterized by in-situ XRD, XPS, H 2 -TPR, NH 3 -TPD, in-situ FT-IR, Raman and TEM. The trend of the initial reaction rate follows: MoO 3 (0.18 μmol∙g cat −1 ∙s −1 ) < Ni/MoO 3 (0.26 μmol∙g cat −1 ∙s −1 ) < Co/MoO 3 (0.29 μmol∙g cat −1 ∙s −1 ), corresponding to the decreasing activation barrier. And the best catalytic activity was observed for the 100% yield of BP over Co/MoO 3 . A possible mechanism, including Co(Ni) facilitated reduction of Mo 6+ to Mo 5+ and Co(Ni) enhanced formation of acidic sites, is proposed to be responsible for the high activity in Co(Ni)/MoO 3 catalysts.
研究领域:
催化化学
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可再生能源
·
材料科学
✓ 已验证
DOI
高影响因子
INTEGRATED FERROELECTRICS
·
2018
·
IF 0.367
Xiaolei Song,Yuan Yu,Chunxia Wang,Mingqiao Ge
Magnetic nanoparticles of Nd-Fe3O4 were prepared by hydrothermal synthesis method, using NdCl3·6H2O and FeCl3·6H2O as the starting materials in this paper. The structure and morphology of nanoparticles were investigated by XRD, FTIR, EDS and TEM. The results showed that, while the addition of Nd at 10% in mole ratio, resulted in the formation of Nd2O3 crystal peak in cubic Fe3O4 nanocrystallites by XRD. The absorption bands of Fe‒O, ‒OH, ‒O‒C‒O‒ and ‒CH2‒ were accordant to the correspondent chemical groups by FTIR. The morphology of the prepared nanoparticles exhibited spherical structure and evenly distributed without agglomeration phenomenon by TEM. The elemental composition were mainly consistent with the precursor materials used in the experiment.
研究领域:
材料科学
·
纳米技术
·
化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2019
·
IF 5.128
Xue-Ke Li,Zhi-Min Zong,Yi-Feng Chen,Zheng Yang,Guang-Hui Liu,Fang-Jing Liu,Xian-Yong Wei,Bao-Jun Wang,Feng-Yun Ma,Jing-Mei Liu
A highly active difunctional Ni-Mg 2 Si/γ-Al 2 O 3 was prepared by thermally decomposing nickel tetracarbonyl onto γ-Al 2 O 3 impregnated with Mg 2 Si. The non-catalytic hydroconversion (NCHC) and catalytic hydroconversion (CHC) of the extract ( E ) and extraction residue (ER) from Yinggemajianfeng lignite were investigated over Ni-Mg 2 Si/γ-Al 2 O 3 at 240 °C in n -hexane. Benzyloxybenzene and oxybis(methylene)dibenzene were used as lignite-related model compounds to speculate the possible mechanisms for the catalytic hydrocracking and hydrogenation over Ni-Mg 2 Si/γ-Al 2 O 3 . As a result, more organic matter in ER was converted to soluble portion (SP) by the CHC than by the NCHC. The main SP from the CHC are chain alkanes and cyclanes, while that from the NCHC is rich in arenes and oxygen-containing organic compounds. The results indicate that Ni-Mg 2 Si/γ-Al 2 O 3 effectively catalyze the hydrocracking of >C alk –O– linkages and the hydrogenation of aromatic rings in E and ER.
研究领域:
化学工程
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 40
·15322-15329
·
IF 4.569
Xinze Du,Chaofeng Zhang,Shenglin Liu
The selective activation of C–O ether bonds is an essential tool in organic synthesis and natural polymer depolymerization. However, the direct cleavage of the ether bond is still challenging work, especially breaking this inert and redox-neutral bond to provide one active carbon radical and another oxygen-centered fragment with oxidation capacity that can participate in the controllable radical reaction. We herein report that commercial 2H-MoS2 with negligible acidity can efficiently catalyze the benzylation of arenes with benzyl ethers, and a new Radical-Friedel–Crafts mechanism is proposed, which is quite different from the strong acid-catalyzed Friedel–Crafts mechanism. With dibenzyl ether as the model benzylation reagent, 2H-MoS2 can achieve the homolytic cleavage of the Bn–OR bond to generate the benzyl carbon radical and RO˙ species, identified by EPR measurement and radical trap experiments. The following radical-involved benzylation is confirmed by the Hammett results and a plausible pathway is proposed to clarify the Radical-Friedel–Crafts process. Heterogeneous 2H-MoS2 can be consecutively used four times without regeneration and it offers 94–95% yields of 2-benzyl-1,4-dimethylbenzene from dibenzyl ether and p-xylene in 30 min at 140 °C. Furthermore, this mechanism can provide some inspiration to activate the ether bond and to utilize ether as an oxidant in C–H bond activation.
研究领域:
有机化学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2023
·
IF 7.4
Lixia Li,Zhechao Huang,Fenghao Shu,Ying Gao,Jinxing Long
Novel techniques for upgrading heavy lignin bio-oil, the phenolic oligomer from lignin depolymerization, are of great significance for achieving better utilization efficiency of carbon element in lignin. In this study, we proposed an efficient approach for producing high-quality oxygen-containing fuel from the renewable lignin bio-oil via the C-O bond cleavage and the subsequent hydrogenation over the Cu and Ni supported on alkaline MgO . Noticeably, the optimized Cu 6 Ni 20 /MgO resulted in inspiring yields of ethylbenzene (88.6%) and cyclohexanol (98.3%) from lignin dimers, and a colorless fuel with a high-heating value of 31.4 MJ kg −1 from the realistic lignin bio-oil. The results of catalyst characterization also unveiled that introducing Cu species reduced the formation of NiMgO x solid solution, which increased the content of Ni 0 and consequently promoted the performance of upgrading lignin bio-oil. Furthermore, the recondensation of phenolic oligomers could be effectively restrained by the alkaline MgO. In addition, a plausible mechanism was proposed. Therefore, this work opens a promising avenue to designing efficient strategies for utilizing the heavy components from lignin depolymerization.
研究领域:
化学工程
·
可再生能源
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2026
·
IF 18.1
Li Xiancheng,Xia Yuangu,Ma Yanchao,Liu Jiaxuan,Ma Yue,Wang Shuizhong,Lu Qiang,Song Guoyong
C-lignin, a natural biopolymer of caffeyl alcohol subunits linked by benzodioxane motifs, is an ideal feedstock for direct catechol production. However, its hydrogenolysis is hindered by the high bond dissociation energies and steric congestion of vicinal C–O bonds in benzodioxane structures. Here, we report a low-loaded Co–Zn dual single-atom catalyst (Co SA –Zn SA @NC) that enables efficient C-lignin hydrogenolysis, achieving 84.6% catechol yield, 82% selectivity toward 4-propylcatechol, and a turnover number five times higher than precious Ru/C, attributing to the synergistic effect of the dual atomic sites. The major product, 4-propylcatechol, can be readily purified and upgraded into diverse value-added molecules. Mechanistic investigations reveal that the Zn and Co species, acting as the directing and active centers, respectively, synergistically drive the quasi-concerted cleavage of the vicinal C–O bonds. This work presents an atomically dispersed non-precious metal catalyst for C-lignin hydrogenolysis, providing a sustainable route to well-defined aromatics.
✓ 已验证
产品关联
DOI
高影响因子
DIAMOND AND RELATED MATERIALS
·
2026
·
IF 5.2
Shihao Zhang,Feng Liu,Lei Ding,Jingjing Qi,Yuzheng Wang,Yuhan Wu,Laishi Li,Xudong Sun,Yusheng Wu
The persistent contamination of aquatic systems by tetracycline antibiotics necessitates the development of efficient and sustainable adsorbents. Herein, a one-step deep eutectic solvent (DES) strategy is developed for the synthesis of carbon/oxygen co-doped hexagonal boron nitride (BCNO) nanosheets, using a ternary DES (H 3 BO 3 /urea/guanidine hydrochloride) as an all-in-one precursor and self-templating medium. The resulting BCNO material exhibits an ultrahigh tetracycline adsorption capacity of 428.5 mg g −1 . In situ pyrolysis analysis combined with theoretical simulations reveals that the DES-guided process facilitates synergistic heteroatom doping and the formation of a hierarchically porous structure enriched with Lewis acid-base sites. The adsorption process follows a multilayer chemisorption mechanism, driven by the concerted contribution of π-π stacking, hydrogen bonding, and Lewis acid-base coordination. The material exhibits excellent regenerability, retaining >85% of its original adsorption efficiency after five consecutive cycles. This work not only presents a scalable and eco-friendly route to functional BN nanomaterials but also provides fundamental insights into the molecular-level design of high-performance adsorbents for environmental remediation.
✓ 已验证
产品关联
DOI
高影响因子
ORGANIC & BIOMOLECULAR CHEMISTRY
·
2022
·Vol. 20
·期 28
·5535-5542
·
IF 3.89
Na Li,Xiao Liu,Mingliang Zhang,Zekun Zhang,Beibei Zhang,Xiaohui Wang,Juan Wang,Pengfei Tu,Yong Jiang,She-po Shi
Prenyltransferases (PTs) play important roles in the biosynthesis and structural diversification of natural products. In the present study, two new PTs were characterized from a medicinal plant Murraya exotica. MePT1 unprecedentedly catalyses the formation of two C-geranylated products 8/6-C-geranylumbelliferone together with a trace product 7-O-geranylumbelliferone from umbelliferone. MePT2 regio-specifically catalyses the formation of C-3 dimethylallylated products from quinolone alkaloids. This is the first report that a plant PT catalyses the simultaneous formation of C- and O-prenylated products, and a plant PT specifically utilizes quinolone alkaloids as prenyl acceptors. The results not only provide important insight into the functional diversity of plant PTs and the biosynthesis of the prenylated coumarins, quinolone and carbazole alkaloids in Murraya plants, but also pave the way for the overproduction of the prenylated coumarins and alkaloids using metabolic engineering approaches.
研究领域:
生物化学
·
植物生物技术
·
生药学
✓ 已验证
DOI
PubMed
高影响因子
ACS Catalysis
·
2023
·
IF 12.9
Shuai Xu,Qi Gao,Ziyan Hu,Yitong Lu,Yanlin Qin,Yuliang Li
The selective breaking of the Cβ–O bond has great potential for the conversion of lignin into high-value aromatic monomers. In the present work, we designed a CdS–SH/TiO2 heterojunction photocatalyst for the efficient selective breaking of the Cβ–O bond. The surface modification of CdS by –SH promoted close contact between the catalyst and lignin and further promoted the Fermi level matching with TiO2. A type-II heterojunction was constructed by CdS–SH and TiO2 nanosheets to enhance the light absorption range and further increase the separation of photogenerated electron–hole pairs, resulting in high catalytic activity. Finally, 85% phenol and 87% acetophenone yields were obtained under mild light irradiation using 2-phenoxy-1-phenylethanol as the model substrate. Several control experiments, along with DFT calculations, indicate that the reaction pathway is more likely to involve the oxidation of Cα–OH to form Cα═O initially, followed by the activation of Cβ–O, which is then reduced to further form aromatic monomers. This work achieves the efficient selectivity of lignin depolymerization and provides a reference for the design of heterojunction photocatalysts in the valorization of lignin.
研究领域:
化学工程
·
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2025
·
IF 5.3
Ajibola T. Ogunbiyi,Wenzhi Li,Leyu Zhu,Amir Hamza,Jingting Jin
Despite lignin’s massive potential for biobased clean fuel production, developing effective catalysts for selectively cleaving its interunit bonds to harness this potential continues to be challenging. In this study, an HZSM-5-supported MoO3 catalyst was developed for a one-pot, hydrothermal kraft lignin depolymerization to maximize liquid fuel yield. A record-high 85.1% yield of petroleum ether-soluble product (a potential gasoline substitute), an unprecedented 45.3% yield of aromatic monomer, and a meager 4.9% char yield (corresponding to a 95.1% lignin conversion) were realized at 300 °C and 24 h in a catalytic transfer hydrogenolysis. The resulting liquid fuel afforded a calorific value of 35.97 MJ/kg, significantly improving over the 25.45 MJ/kg in the original kraft lignin. Catalyst characterization results showed that an optimal acidity characteristic and a suitable Mo-zeolite interaction were pivotal to the efficient cleavage of the C–O and C–C bonds in the kraft lignin. The analyses of the spent catalyst revealed that the formation of inactive Mo4+ species and carbonaceous deposits on the catalyst’s surface was responsible for the initial catalyst deactivation, but recalcination reinstated the catalyst activity. This study extends the frontiers of knowledge in rational catalyst development for lignin valorization applications.
研究领域:
催化化学
·
生物质能
·
可再生能源
✓ 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）