INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2023
·
IF 8.2
Ying Kang,Xingmei Lu,Junli Xu,Qing Zhou,Guangjin Zhang,Jiayu Xin,Dongxia Yan,Ibrahim E.I. Tantawy E.I. Sayed
Transforming lignin into aromatic monomers is critically attractive to develop green and sustainable energy supplies. However, the usage of the additional catalysts like metal or base/acid is commonly limited by the caused repolymerized and environmental issues. The key step is to mediate electron transfer in lignin to trigger lignin C-C/C-O bonds cleavage without the catalysts mentioned above. Here, we report that the ionic liquids [BMim][ClO 4 ] was found to trigger lignin electron transfer to cleave the C-C/C-O bonds for aromatic monomers without any additional catalyst. The proton transfer from [BMim] + to [ClO 4 ] − could polarize the anion and decrease its structure stability, upon which the active hydroxyl radical generated and induced lignin C-C/C-O bonds fragmentation via free radical-mediated routes with the assistance of photothermal synergism. About 4.4 wt% yields of aromatic monomers, mainly composed of vanillin and acetosyringone , are afforded in [BMim][ClO 4 ] under UV-light irradiation in the air at 80 °C. This work opens the way to produce value-added aromatic monomers from lignin using an eco-friendly, energy-efficient, and simple route that may contribute to the sustainable utilization of renewable natural resources.
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PubMed
高影响因子
Small
·
2023
·Vol. 20
·期 3
·2304990
·
IF 13.3
Na Ye,Wenchao Sheng,Riguang Zhang,Binhang Yan,Zhao Jiang,Tao Fang
The splitting of the C–C bonds of ethanol remains a key issue to be addressed, despite tremendous efforts made over the past several decades. This study highlights the enhancement mechanism of inexpensive NbN-modified Pd 1 Sn 3 -NbN/C towards the C–C bonds cleavage for alkaline ethanol oxidation reaction (EOR). The optimal Pd 1 Sn 3 -NbN/C delivers a catalytic activity up to 43.5 times higher than that of commercial Pd/C and high carbonate selectivity (20.5%) toward alkaline EOR. Most impressively, the Pd 1 Sn 3 -NbN/C presents good durability even after 25 200 s of chronoamperometric testing. The enhanced catalytic performance is mainly due to the interfacial interaction between PdSn and NbN, demonstrated by multiple structural characterization results. In addition, in situ ATR-SEIRAS (Attenuated total reflection-surface enhanced infrared absorption spectroscopy) results suggest that NbN facilitates the C–C bonds cleavage towards the alkaline EOR, followed by the enhanced OH adsorption to promote the subsequent oxidation of C1 intermediates after doping Sn. DFT (density functional theory) calculations indicate that the activation barriers of the C–H bond cleavage in CH 3 CH 2 OH, CH 3 CHOH, CH 3 CHO, CH 3 CO, CH 2 CO, and the C–C bond cleavage in CH 3 CO, CH 2 CO, CHCO are evidently reduced and the removal of adsorbed CH 3 CO and CO becomes easier on the PdSn-NbN/C catalyst surface.
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PubMed
高影响因子
Nature Communications
·
2026
·
IF 18.1
Wang Wei,Tang Yonghua,Su ZhuiZhui,Liu Huanmin,Liu You-Nian,Tang Dingguo,Zhou Peng
Photocatalytic carbon–carbon coupling offers a route for converting plastic-derived chemicals into valuable multi-carbon products, yet uncontrolled coupling of intermediate limits efficiency and selectivity. Here, we report atomically dispersed barium species on titanium dioxide that act as frustrated Lewis pairs, enabling efficient and selective generation intermediates during the co-oxidation of ethylene glycol and methanol toward lactic acid. The barium species create interstitial states near the Fermi level, enhancing charge separation and surface redox activity. Meanwhile, barium sites promote the formation of transient •CHOHCH 2 OH radicals from ethylene glycol, while lattice O generates stable *CH 3 intermediates from methanol. Their directed cross-coupling yields lactic acid at rate of 2.04 ± 0.08 mmol g –1 h –1 with 81.8 ± 2.4 % carbon selectivity, alongside H 2 evolution at 5.85 ± 0.23 mmol g –1 h –1 . In this work, we show an alkaline-earth frustrated Lewis pairs for selective solar-driven cross-coupling reaction.
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PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Zhizhou Cai,Ning Cao,Fanxing Zhang,Xiangzhou Lv,Ke Wang,Yi He,Yao Shi,Hao Bin Wu,Pengfei Xie
Electrocatalytic CO 2 reduction into ethanol driven by renewable energy represents a promising strategy for energy storage and mitigation of global warming, but it has remained challenging to gain high activity and selectivity of ethanol. Here we take advantage of atomic arrangement in immiscible Ag-Cu composite during annealing and establish hierarchical interfaces in the obtained core-shell catalyst. The atomic Ag-Cu interactions increase electrochemical surface area and expedite charge dynamics, resulting in an unprecedented electrocatalytic performance with the faradaic efficiency of C 2+ products, ethanol as 80.2 %, 52.6 % and the current density of ∼320 mA cm −2 at −1.0 V (versus reversible hydrogen electrode). Moreover, the Ag-Cu catalyst exhibits a notable stability for ∼60 h. Mechanism studies reveal that local CO intermediates preferentially accumulate on the core, then migrate to the continuous Cu surface for C-C coupling energy-favorably toward ethanol. Our work highlights a novel design principle as interface engineering for advanced tandem electrocatalysts.
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高影响因子
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2023
·
IF 5.7
Zhenxiao Tang,Maozhong Yi,Zhe Zhou,Huang Wu,Yuanming Zhou,Ke Peng
A C/C-TaB 2 -SiC composite was successfully prepared by high-solid-loading slurry impregnation combined with polymer infiltration and pyrolysis. The composite had a density of 3.46 g/cm 3 and consisted of pyrolyzed carbon, carbon fibers, TaB 2 particles, and precursor-derived SiC with their mass fractions of 7.8 %, 13.0 %, 58.6 %, and 20.6 %, respectively. The C/C-TaB 2 -SiC composite possessed a flexural strength of 248.2 ± 16.8 MPa and a fracture toughness of 13.7 ± 1.6 MPa·m 1/2 , and demonstrated a non-brittle fracture behavior . After exposure to oxyacetylene flame with a heat flux of 4.18 MW/m 2 for 120 s, the ablation temperature of the sample surface reached a maximum of 2263 °C, and the mass and line ablation rates were 2.24 mg/s and 12.92 µm/s, respectively. The ablation resistance mainly comes from the hindrance of oxygen diffusion by the oxide layer composed of tantalum oxide and a small amount of SiO 2 .
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Wen Zhang,Yingxiu Zhao,Jiayi Li,Yu Miao,Pengkai He,Zexing Wu,Yang Zhang,Guang-Rui Xu,Lei Wang
The capacity of C‒C bond cleavage determines the pathway selectivity during the ethanol oxidation process. Herein, ultra-thin monodisperse PdCo nanosheets with an average diameter of 33 nm are successfully synthesized and the interface of Pd-O-Co is further constructed due to the introduction of lattice oxygen. Due to their ultra-thin nanosheet structure, unique surface electronic structures driven by lattice oxygen, and alloying effect, the prepared PdCo/Pd-O-Co nanosheets (PdCo/Pd-O-Co NSs) show excellent ethanol oxidation reaction (EOR) activity and stability. The mass activity and specific activity of PdCo/Pd-O-Co NSs are 12.43 A mg −1 and 22.01 mA cm −2 for EOR, which exceeded PdCo nanosheets, Pd nanosheets and commercial Pd black. In situ FTIR spectroscopy and theoretical calculation identified that lattice oxygen introduced after square-wave potential treatment can promote the cleavage of the C‒C bond. Through the introduction of lattice oxygen combined with lattice strain engineering, the PdCo/Pd-O-Co NSs surface is optimized to promote the generation of strong p-d orbital hybridization, which led to the upward shift of the d-band center and the electron delocalization effect, effectively promoting the C‒C bond cleavage and improving the anti-poisoning ability.
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高影响因子
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2025
·
IF 6.2
Yuanming Zhou,Shuxin Li,Shuangxing Zhu,Ruizhi Liu,Zhenxiao Tang,Maozhong Yi,Ke Peng
To investigate the influence of (Ta,Zr)C on the ablation resistance of C/C composites, C/C-(Ta 0.5 Zr 0.5 )C-SiC, C/C-(Ta 0.33 Zr 0.67 )C-SiC, and C/C-(Ta 0.2 Zr 0.8 )C-SiC were prepared with different Zr/Ta ratios through high-solid-loading slurry impregnation combined with precursor infiltration and pyrolysis. The flexural performance and ablation resistance both improved with an increasing Zr/Ta ratio. Compared to C/C-(Ta 0.5 Zr 0.5 )C-SiC and C/C-(Ta 0.33 Zr 0.67 )C-SiC, the flexural strength of C/C-(Ta 0.2 Zr 0.8 )C-SiC increased by 74.17 % and 24.29 %, respectively. The mass ablation rate was reduced by 74.33 % and 81.02 %, while the linear ablation rate was reduced by 98.60 % and 97.65 % after 120 s of ablation, respectively. The variations in Zr/Ta ratios affected the formation, integrity, and performance of the microstructure, which was composed of a Zr-rich oxide skeleton combined with Ta-rich oxide binder within the Ta-Zr-O oxide layer on the composite surface, ultimately enhancing the overall ablation resistance of these composites.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Tiantian Wang,Jianhong Wei,Furong Shi,Hejie Wang,Jinye He,Xudong Lv,Yuan Zhou,Pengzhi Guo,Chenglong Wang,Yangjun Xia
In recent years, polymerized small molecule acceptors (PSMAs) have emerged as a promising strategy that combines the strong absorption of small molecules with the film-forming ability and stability of polymers, thereby greatly boosting the performance of all-polymer solar cells (all-PSCs). We designed a non-fused acceptor, DTBT-IC, and its polymeric counterpart, PDTBT-Br-T, by selecting DTBT as the core, bithiophene as the π-bridge, and IC as the terminal group. PDTBT-Br-T was synthesized via Stille coupling and used with PM6 as the donor to fabricate organic solar cells. The PDTBT-Br-T-based device delivered superior performance, with a VOC of 1.050 V, JSC of 9.32 mA cm−2, FF of 45.33%, and a PCE of 4.44%, outperforming the DTBT-IC-based counterpart. Morphological and structural analyses revealed that PDTBT-Br-T exhibits more ordered backbone stacking and defined phase separation, enhancing exciton dissociation and charge transport, and suppressing energy loss. The study highlights that polymerization of DTBT-IC enhances intermolecular packing and microstructure, offering critical design insights for efficient all-PSCs.
研究领域:
材料科学
·
高分子化学
·
有机电子学
·
光伏技术
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DOI
高影响因子
ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Bao Liu,Chao Cai,Baopeng Yang,Kejun Chen,Yan Long,Qiyou Wang,Shuandi Wang,Guozhu Chen,Hongmei Li,Junhua Hu,Junwei Fu,Min Liu
Electrochemical carbon dioxide (CO 2 ) reduction reaction (CO 2 RR) to obtain C2/multi-carbon fuels is an appealing technology to reduce carbon emission and store intermittent renewable electricity. The C–C coupling process, as the most critical step for generating C2/multi-carbon fuels, strongly depends on the concentration of *CO intermediates around the active sites. In this work, we prepared porous copper nanospheres (P-Cu) that greatly improved the C–C coupling process by enriching *CO intermediates in the pore structure . The specific pore features of P-Cu were characterized in detail by scanning electron microscopy (SEM), transmission electron microscopy (TEM), and nitrogen adsorption/desorption tests. Obviously, the P-Cu exhibits higher specific surface area and richer pore structure than the control sample compact copper nanosphere (C-Cu). The CO gas sensor and temperature programmed desorption (TPD) tests prove that the P-Cu has better CO adsorption and enrichment capacity than C-Cu due to the rich pore structure. As a result, P-Cu exhibited a high C2 selectivity with a Faradaic efficiency (FE C2 ) of 57.22% at −1.3 V ( vs . RHE), which is about 2.5-fold than the C-Cu (FE C2 of 22.71%). This work provides an effective strategy to improve the activity and selectivity of C2 products in CO 2 RR by optimizing the adsorption/enrichment property of intermediates.
研究领域:
材料科学
·
能源化学
·
催化化学
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
ShiWen Luo,ChengWei Deng,Kan Zhang,Sheng Zhu,QunJie Xu,YuLin Min
Reasonable interface regulation is a promising way to obtain bifunctional or multi-functional catalysts as the heterogeneous interface generally offers unique electronic structures. Here, we design a strongly coupled interface structure in Ni 3 Mo 3 N/Mo 2 C coated with graphitized carbon (Ni 3 Mo 3 N/Mo 2 C@C) by using an in-situ growth strategy. The density functional theory calculation unveil that the heterointerface of Ni 3 Mo 3 N/Mo 2 C@C not only facilitates the charge transfer, but also regulates the adsorption free-energies of the reaction intermediates (*O, *OH, and *OOH), to achieve superior electrocatalytic performances for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). As bifunctional catalysts, the Ni 3 Mo 3 N/Mo 2 C@C exhibits high HER and OER activities, with 43 mV and 220 mV overpotentials at the current density of 10 mA cm −2 in 1 M KOH electrolyte, respectively, as well as outstanding catalytic durability. This interface coupling strategy may provide a useful path to promote the electrocatalytic activities for diverse reactions in the energy field.
研究领域:
材料科学
·
能源科学
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高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Yan Li,Guangyu Chen,Jie Lin,Liuqing Huang,Chentong Zhang,Xuetao Luo
TC4 (Ti–6Al–4V) nanoparticles (TC4NPs) and silicon nanoparticles (SiNPs) with a median size of 146 and 51 nm were prepared by sand milling from scrap produced by refining silicon and TC4. The SiNPs and TC4NPs are mixed, carbonized, and leached in different proportions to obtain Si@C/TiO2@C/Hollow-C anode materials. The special structure of the anode materials provided more space for the volume expansion of silicon. The anatase TiO2 in TC4NPs relieves the volume expansion and reduces the transfer impedance, and the lithiated TiO2 can promote the electrical conductivity of the Si@C/TiO2@C/Hollow-C anode during the charge/discharge process. Furthermore, the Si@C/TiO2@C/Hollow-C (SiNPs/TC4NPs = 2:1) electrode delivers excellent rate performance; after cycling at a series of higher current densities, 92% of the original level of the reversible capacity can be maintained. The Si@C/TiO2@C/Hollow-C (SiNPs/TC4NPs = 2:1) anode retains 558 mA h·g–1 after 400 cycles with a large current density of 1000 mA·g–1. The synthesis method of the Si@C/TiO2@C/Hollow-C anode is a low-cost, facile, and nontoxic process, endowing it with the potential for application as energy materials for mass production.
研究领域:
材料科学
·
能源技术
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高影响因子
Catalysis Science & Technology
·
2023
·Vol. 13
·期 6
·1748-1754
·
IF 5
Shaoyuan Guo,Xinli Tong,Lingwu Meng,Guobao Yang
Selective oxidative C–C and C–O bond cleavage is of significance to the efficient utilization of biomass and biomass-derived platform compounds. In this work, the selective oxidative cleavage of C–C and C–O bonds has been developed with an iron-based catalyst (Fe–N–C) in the presence of molecular oxygen. Specifically, the β-O-4 lignin model compound was successfully converted to phenol and methyl benzoate in a methanol solvent, where the substrate conversion was 95.0% and the yields of phenol and methyl benzoate were 94.9% and 63.7%, respectively, when the reaction was performed with the Fe–N–C-850 catalyst at 120 °C for 4 h. Also, the oxidative transformations of other lignin models to phenols and methyl benzoates were achieved. Further investigations showed that the existence of the Fe3C phase in the catalyst plays an important role in the aerobic oxidative cleavage of C–C and C–O bonds in the β-O-4 lignin model.
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