GREEN CHEMISTRY
·
2021
·Vol. 23
·期 13
·4741-4752
·
IF 10.182
Song Li,Qiaozhi Ma,Wenxin Zhong,Xuelai Zhao,Xiangqian Wei,Xinghua Zhang,Qiying Liu,Chenguang Wang,Longlong Ma,Qi Zhang
Catalytic hydrodeoxygenation of bioderived furans is critically attractive to prepare sustainable fuels. Herein, a novel octanediol-route was developed to produce octane through one-pot conversion of bioderived furans at low temperatures. A 96.6% yield of octane was obtained by catalytic conversion with Pd/C and phosphotungstic acid (HPW). Experimental validation of the novel pathway revealed that octanediol intermediates could be formed through hydrogenolysis of furans before deoxygenation. The spontaneous process of this octanediol-route was thermodynamically confirmed by DFT simulations. In addition, characterization studies suggested that water in the system strengthened the cooperation between metals and acids to facilitate C–O bond scission through the modification and hydrogen transfer of HPW. This work highlights a promising reaction pathway for an efficient HDO catalytic system to obtain alkanes from bioderived furans under mild conditions.
研究领域:
催化
·
可持续化学
·
可再生能源
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高影响因子
JOURNAL OF CATALYSIS
·
2020
·
IF 7.888
Yanru Zhu,Jian Zhang,Xiaodan Ma,Zhe An,Shaowei Guo,Xin Shu,Hongyan Song,Xu Xiang,Jing He
Complexity of chemical linkages (C-C/C-H/C-O, C=C/C=O, or C-O-H/C-O-C) in biomass-derived molecules makes the selective activation of targeted bonds much more challenging, expecting well-defined catalysts and definite catalytically-active sites. This work demonstrates an effective gradient reduction strategy to control the definite structure of catalytically-active sites, affording defects-rich nano-twin Cu particles. This strategy just involves the reduction (calcination under H 2 ) of Cu II -containing layered double hydroxides (LDHs) simply with controlling the reduction gradient (interval time) of Cu II species in two chemical micro-environments (Cu II -O-Cu II and Cu II -O-M II/III/IV (M ≠ Cu)) in the brucite-like layer of LDHs. The nano-twin Cu particles efficiently promote the target activation of C-O and C=C in the conversion of furfural to cyclopentanone (CPO). With ~100% furfural conversion, the defects-rich nano-twin Cu particles afford a CPO selectivity of 92%, 50% higher than regular spherical Cu particles. The multi-stepped defect sites, originating from the planar defects, play a decisive role in promoting the CPO selectivity by facilitating the hydro-deoxygenation to C-O of 4-hydroxycyclopentenone (HCP) and hydrogenation to C=C of HCP or cyclopentenone.
研究领域:
催化化学
·
材料科学
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DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2026
·
IF 17.2
Chongzheng Xu,Haoping Di,Fengyue Sun,Wenjing Bao,Yanwei Ju,Dengwei Yan,Changle Yue,Yiyuan Xu,Yunxiu Zhao,Shuo Wang,Jiqian Wang,Yukun Lu
Sulfided NiMo catalysts can effectively hydrogenate oxygen-rich bio-oils into high quality hydrocarbon fuels. However, precisely controlling the cleavage of C−O bonds remains challenging. Here, we synthesized an oil-soluble precursor NiMo 6 -DODA by encapsulating the polyoxometalates (POMs) (NH 4 ) 4 [NiMo 6 O 24 H 6 ] (NiMo 6 ) with surfactants, followed by in-situ construction of an ultra-dispersed monolayer NiMoS catalyst. The “surfactant shell” of the precursor ensured its homogeneous dispersion in the oil phase, while gradually sacrificing and decomposing during the sulfidation to mitigate the aggregation of the MoS 2 nanosheets. Meanwhile, the well-defined “POMs core” established an atomic-level Ni-Mo proximity, ensuring the dominance of the Ni-promoted MoS 2 active phase. This design not only altered the adsorption configuration of esters on the NiMo catalyst but also introduced abundant edge sulfur vacancies to promote oxygen atom adsorption and accelerate C−O bond cleavage. The results showed that NiMo 6 -DODA achieved 100% conversion of methyl palmitate and 100% alkane selectivity under low catalyst loading conditions. Notably, the selectivity for n -hexadecane reached 94.2%, significantly surpassing that obtained with a commercial oil-soluble precursor (69.8%). Furthermore, the catalyst maintained high activity across multiple reaction cycles and in the solvent-free conversion of real bio-oils. This strategy of pre-assembly combined with sacrificial sulfidation provides a simple and effective route for designing hydrodeoxygenation catalysts that enable precise control over ester C−O bond cleavage.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Hong Li,Xinzhu Wen,Feng Shao,Shiwei Xu,Chao Zhou,Yafei Zhang,Hao Wei,Nantao Hu
Rational materials design is critical to develop advanced electrodes for high-performance sodium-ion battery. In this work, a well-designed structure with interlayer-expanded molybdenum disulfide (MoS 2 ) vertically anchored on graphene substrates (v-MoS 2 /rGO) is achieved by one-pot hydrothermal synthesis . The vertical anchored MoS 2 and high conductivity graphene sheets provide a good path for electrons/ion transfer. More importantly, the direct linkage of O from functional group on graphene oxide (GO) with edge S of MoS 2 (C-O-S) is constructed, which can maintain the stability of the v-MoS 2 /rGO electrode and enhance its electrons transport rate for the high-rate performance and long cycle life. The assembled sodium-ion battery shows high rate performance (129.2 mAh g −1 at 10 A g −1 ) and long cycling stability (251.2 mAh g ‐1 −1 at 2 A g −1 after 1000 cycles with an ultra-low degradation of 10.9 μAh g −1 per cycle). The excellent performance makes the designed structure a fascinating anode for sodium battery.
研究领域:
材料科学
·
能源存储
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DOI
高影响因子
MACROMOLECULES
·
2020
·
IF 5.918
Fan Zhang,Tiantian Li,Wanting Chen,Xiaoming Yan,Xuemei Wu,Xiaobin Jiang,Yang Zhang,Xiaozhou Wang,Gaohong He
As critical triggers, both the electron-withdrawing links and neighboring cationic groups induce and accelerate the aryl ether cleavage in the widely used aryl ether containing anion exchange membranes (AEMs). Herein, a novel alkaline stable polyelectrolyte is proposed by converting the electron-withdrawing C═O links in the widely used poly(aryl ether ketone) backbone into the electron-donating C–NH2 links, and then grafting faraway para-type cations by Leuckart-Menshutkin reaction without using noble metal catalysts. Contributions of the elimination of electron-withdrawing C═O links and graft of para-type cations to the excellent alkaline stability of the aryl ether containing polyelectrolytes are demonstrated through density functional theory, as the increasing electron cloud density on the ether-connected carbon atom elevates the activation energy barrier to OH– initiated aryl ether cleavage, and the para-type cation is more stable than the conventional ortho-type cation due to the sterical protection and low electrophilicity to benzylic carbon. By converting C═O to C–NH2 groups and then tuning the quaternization degree, the remaining C–NH2 groups in the polymer backbone could form hydrogen bonding networks to reinforce the membranes. The novel quaternized poly(aryl ether amine) membrane exhibits high conductivity (92.2 mS cm–1 at 80 °C), excellent mechanical properties (48.2 MPa, 51.3%), and suppressed swelling ratio (12.8% at 80 °C). Excellent alkaline stability is also confirmed experimentally with no polymer backbone degradation even in harsh conditions (4 M KOH, 80 °C, 400 h), which is at the top level among the state-of-the-art side chain and aryl ether-free types of AEMs.
研究领域:
材料科学
·
化学工程
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高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2023
·
IF 8.7
Chen Yang,Jian Yang,Shuangshuang Liu,Mingxue Zhao,Xu Duan,Hongli Wu,Lang Liu,Weizao Liu,Jiangling Li,Shan Ren,Qingcai Liu
Owing to its feasibility, efficiency in light-harvesting and effectiveness in the interfacial charge transfer between two n-type semiconductors, constructing heterojunction photocatalysts have been identified as an effective way for enhancing the photocatalytic properties. In this research, a C–O bridged CeO 2 /g-C 3 N 4 (cCN) Step-scheme (S-scheme) heterojunction photocatalyst was constructed successfully. Under visible light irradiation, the cCN heterojunction exhibited the photocatalytic degradation efficiency of methyl orange, which was about 4.5 and 1.5 times higher than that of pristine CeO 2 and CN, respectively. The DFT calculations, XPS and FTIR analyses demonstrated the formation of C–O linkages. And the calculations of work functions revealed the electrons would flow from g-C 3 N 4 to CeO 2 due to the difference in Fermi levels , resulting in the production of internal electric fields . Benefiting from the C–O bond and internal electric field, the photo-induced holes in the valence band of g-C 3 N 4 and the photo-induced electrons from conduction band of CeO 2 would be recombined when exposed to visible light irradiation, while leaving the electrons with higher redox potential in the conduction band of g-C 3 N 4 . This collaboration accelerated the separation and transfer rate of photo-generated electron-hole pairs, which promoted the generation of superoxide radical (•O 2 − ) and improved the photocatalytic activity .
研究领域:
材料科学
·
环境科学
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DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Hongyu Qu,Xiangcheng Li,Xiao Han,Junjie Li,Xinqiang Feng,Chuang Liu,Zhendong Wang,Weimin Yang
Rational design of highly efficient non-noble-metal catalysts for the selective hydrogenolysis of biomass platform compounds to produce fuels and fine chemicals is a key pursuit for the sustainable chemical industry. In this work, we report for the first time the synthesis of a Ni-supported germanosilicate zeolite (Ni-SCM-14) catalyst by a simple grinding method, showing both satisfactory yield (90.3%) and good stability in eight cycles for the hydrogenolysis of 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF). Characterization revealed that Ni nanoparticles were highly dispersed on the SCM-14 zeolite with strong interactions. The synergistic effect of highly dispersed Ni hydrogenation sites and the weak acidity activation of the C–O bond provided by SCM-14 is considered to be the key to the efficient hydrogenolysis of HMF. This discovery opens up a new avenue for germanosilicate zeolite to activate the C–O bond.
研究领域:
催化化学
·
生物质转化
·
材料科学
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DOI
高影响因子
AICHE JOURNAL
·
2025
·
IF 4
Jinlin Mei,Zhentao Liu,Zhengkai Cao,Aocheng Wang,Xiaoyang Kong,Aijun Duan,Chunya Wang,Chunming Xu,Xilong Wang
Hierarchical Y/SBA-15 meso-microporous composites (YS- x ) and corresponding highly dispersed catalysts (Ni/YS- x ) were prepared and applied to the production of jet fuel range hydrocarbons by the selective hydrogenation of oleic acid. Small particle size and electron-deficient Ni δ+ are detrimental to the C C bond activation of the η 1 (C)-acyl conformation and inhibit the decarbonylation/decarboxylation pathway. Besides, the activation ability of the C C bond is regulated to avoid excessive cleavage by the acidity and diffusion properties of the hierarchical Ni/YS- x catalysts, thus affecting their hydroisomerization and hydrocracking properties. The abundant acid sites are beneficial to the selective activation of the C O bond of the η 2 (C, O)-aldehyde conformation and the promotion of the reductive deoxygenation pathway. The optimal Ni/YS-1 shows the highest iso / n -alkane ratio ( i / n = 6.26) and superior jet fuel range hydrocarbons yield (48.8%, 340°C), which is a benefit from its outstanding acid–metal balance and worthy diffusion property.
研究领域:
催化
·
多孔材料
·
化学反应工程
·
能量转换
·
表面化学
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Zhuoran Song,Daohu Sheng,Siyao Cheng,Mengmeng Zhang,Aming Xie
The development of two-dimensional (2D) metal composite materials for electromagnetic wave (EMW) absorption is hindered by complex fabrication processes, high raw material costs, and insufficient absorption performance. We ingeniously integrate a multi-metal doping strategy with the oxygen-rich two-dimensional structure of p(C₃O₂)ₓ to successfully construct a defect-rich two-dimensional metal composite microwave absorber. Spectroscopic analysis reveals that multi-metal doping and oxygen release during pyrolysis generate abundant heterogeneous interfaces (oxides/alloys) and induce pronounced electron delocalization, promoting lattice distortions and defect formation. This synergistic effect significantly enhances both local dipole and interfacial polarization, boosting dielectric response. Consequently, the optimized OC-FeMnCuCo sample achieves exceptional EMW absorption with a minimum reflection loss (RL min ) of –55.0 dB and a broad effective absorbing bandwidth (EAB) of 6.8 GHz at an ultra-thin thickness of 1.9 mm. CST simulations further confirm its practical applicability. This work provides a simple, cost-effective strategy for designing advanced 2D absorbers.
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高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2026
·
IF 6.4
Zheyuan Ding,Juncheng Zhao,Jiaming Zhang,Junzhong Xie,Kunye Zhang,Cenkai Zhao,Jikun Xu,Yu Wang,Xuepin Liao,Xiao Xiao,Bi Shi
A 100% lignin β -O-4 model conversion with 93.1% monomer selectivity and a high TON was obtained. • The interplay between Ru particle and single atom contributed to the high performance. • Favorable stability under high-temperature heating and high-pressure with reusability > 97%. Catalytic hydrogenolysis is a promising strategy for converting lignin into valuable aryl platform chemicals, contingent upon the availability of high-performance catalysts. The philosophy for the catalyst rational design towards high conversion and selectivity was rarely reported to the best of our knowledge. We illustrate the synergistic interplay between Ru particles and single atoms, contributing to the high catalytic performance. The N-doped carbon-supported Ru catalyst is designed by combining collagen fiber-immobilized tannin adsorption with carbonization (TNC). The Ru is finely dispersed on the TNC support in the form of both single atoms and nanoparticles at a low metal loading of 0.91 wt% (noted as Ru/TNC). It achieved a 100% conversion with a 93.1% aromatic monomer yield in the catalytic hydrogenolysis of lignin β –O–4 model 2-phenoxy-1-phenylethanol (PPE) at 260 °C and 2 MPa H 2 . The primary products of this reaction included ethylbenzene, cyclohexanol, and ethylcyclohexane, and a high turnover number (TON) of 955 was obtained, which surpassed most reports. Specifically, the Ru particle sites facilitate efficient H 2 dissociation, while the single-atom sites provide a weakly adsorbing environment for reaction intermediates due to electron-rich isolated Ru atoms, thereby effectively suppressing over-hydrogenation. This work offers a promising catalyst rational design principle for selective hydrogenation for efficient C–O bond cleavage of lignin, demonstrating significant potential in transforming lignin into value-added platform chemicals. Download: Download high-res image (151KB) Download: Download full-size image Possible reaction pathway on Ru/TNC catalyst consisting of Ru particle and Ru single atom. The intermediates easily desorbed over Ru single atom site due to the weak adsorption. Purple ball: Ru atom, red ball: N atom, white ball: H atom where Ru particles serve as H* species supply pump due to H spillover.
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高影响因子
ENERGY & FUELS
·
2026
·Vol. 40
·期 33
·18068-18080
·
IF 6
Fu Zong-Pin,Zhao Yun-Peng,Wu Yu-Fa,Qiu Le-Le,Liu Fang-Jing,Zhong Mei,Liang Jing,Cao Jing-Pei
Efficient depolymerization of lignite remains challenging
owing
to both its structural complexity and the high stability of oxygen-containing
bridge linkages. Herein, low-temperature pyrolysis and oxidative pretreatments
were employed to regulate oxygen-containing structures and enhance
the hydrogenolysis reactivity of Zhaotong lignite (ZT). These pretreatments
promoted the structural evolution of lignite, activated oxygen-containing
bridge structures, and suppressed the recondensation of reactive intermediates,
thereby facilitating subsequent depolymerization reactions. A CuCoOx
catalyst capable of dynamic in situ reconstruction was introduced
for catalytic hydrogenolysis. Under reaction conditions, partial reduction
of CuCoOx generated reconstructed Cu 0 -CoOx interfacial
active sites, where the synergistic interaction between metallic Cu
and defect-rich CoOx promoted H 2 activation and selective
C–O bond cleavage. Density functional theory (DFT) calculations
further revealed that interfacial electron redistribution at the Cu
cluster/Vo-Co 3 O 4 (311) interface facilitated
H 2 activation and stabilized reactive hydrogen species.
These findings provide new mechanistic insights into pretreatment-regulated
and interface-controlled hydrogenolysis pathways for the efficient
valorization of low-rank coal.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Zidan Zou,Zhuoya Chai,Jia Zhang,Chun Chen,Yunxia Zhang,Haimin Zhang,Huijun Zhao,Guozhong Wang
Developing efficient catalysts for selective C═O hydrogenation remains challenging due to the thermodynamic preference for C═C bond activation in α,β-unsaturated aldehydes. To address this limitation, we engineered Pt1Co10 nanoalloys within ethylenediamine-functionalized mesoporous silica (MS) by marrying vacuum-assisted impregnation with spatially constrained self-assembly. This dual spatial–temporal control strategy can achieve precise charge redistribution at metal interfaces, geometric confinement suppressing Ostwald ripening, and optimal hydrogenation pathways via hierarchical porosity. Under industry-feasible conditions (25 °C, 0.5 MPa H2), the Pt1Co10/MS system delivers 96.8% cinnamaldehyde conversion with 72.1% cinnamyl alcohol yield, outperforming conventional Pt or Co catalysts. More importantly, the MS framework’s strain accommodation capability enables activity retention over the cycle test, and the electronic synergy between Pt and Co can optimize adsorption energetics to suppress competitive C═C hydrogenation pathways. This work establishes an approach of bimetal synergy for steering adsorbed intermediate configurations, offering universal strategies for selective hydrogenation catalysis.
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高影响因子
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