JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2025
·
IF 14.3
Junjie Xu,Wei Sun,Xiang Xiong,Yi Zeng,Qingbo Wen
Conventional ultra-high-temperature ceramic-modified carbon/carbon composites (C/C-UHTCs) face limitations such as excessive erosion in the gas environment of solid rocket motors (SRMs). In contrast, metal-reinforced C/C-UHTCs exhibit enhanced mechanical properties, thermophysical characteristics, and resistance to high-temperature erosion. These advantages indicate significant potential for metal-reinforced C/C-UHTCs to augment the thrust capabilities of SRMs. This study demonstrated the preparation of (Hf, Zr, Ti)C-(Hf, Zr, Ti)B 2 -W-Cu cermet modified C/C composites using slurry infiltration and reactive melt infiltration at 1400°C. The microstructure, formation mechanisms, mechanical properties, and thermophysical properties of C/C-(Hf, Zr, Ti)C-(Hf, Zr, Ti)B 2 -W-Cu composite materials, as well as the ablation behavior of the composite materials under the SRM environment were compared. The results showed that the linear and mass ablation rates of the C/C-(Hf, Zr, Ti)C-(Hf, Zr, Ti)B 2 -W-Cu composite material decreased by 112.1% and 160.4% (0.074 mm s −1 , 0.086 g s −1 ), respectively, compared with those of the C/C-(Hf, Zr, Ti)C composite material. This could be attributed to the formation of a dense, high-strength W-skeleton composite (Hf, Zr, Ti)O 2 oxide layer during the ablation of the C/C-(Hf, Zr, Ti)C-(Hf, Zr, Ti)B 2 -W-Cu composite, which effectively resisted erosion from high-temperature, high-speed and high-particle-concentration two-phase gas flow. This work presents a novel approach to enhancing the ablation resistance of C/C-UHTCs and holds significant promise for the development of structural materials in SRM environments.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
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IF 20.2
Kangwang Wang,Mingjie Wu,Peifeng Yu,Hector F. Garces,Ying Liang,Longfu Li,Lingyong Zeng,Kuan Li,Chao Zhang,Kai Yan,Huixia Luo
Despite ongoing research, the rational design of non-trivial topological semimetal surface states for the selective photocatalytic CO 2 conversion into valuable products remains full of challenges. Herein, we present the synthesis of lattice-matched 1 T-OsCoTe 2 for the photoreduction upgrading of CO 2 to tri-carbon (C 3 ) alkane (propane, C 3 H 8 ) by the integration of experimental work and theory prediction/calculation. Experimental studies suggested a high electron-based selectivity of 71.2 % for C 3 H 8 and an internal quantum efficiency of 54.6 % at 380 nm. In-situ X-ray photoelectron spectroscopy and X-ray absorption fine structure spectroscopy demonstrated that Co and Os atoms coordinated with Te atoms enable an efficient Os―Te―Co electron transfer to activate the generation of *CH 3 , *CHOCO and *CH 2 OCOCO. Density functional theory calculations further confirmed Os―Te―Co electron bridging on the improved CO 2 conversion kinetics. To our knowledge, this is the first report suggesting the role of Os atoms in accelerating the photocatalytic CO 2 conversion activity of the topological semimetal 1 T-OsCoTe 2 .
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Wenjie Li,Lifen Li,Qineng Xia,Song Hong,Lijun Wang,Zhibo Yao,Tai-Sing Wu,Yun-Liang Soo,Hao Zhang,Tsz Woon Benedict Lo,Alex W. Robertson,Qingya Liu,Leiduan Hao,Zhenyu Sun
Electrochemical CO 2 reduction (ECR) to commodity chemicals offers a promising way for mitigating the greenhouse effect and driving the transition from fossil-fuel dependence to a sustainable economy. To this end, the design and development of active and robust electrocatalysts is key. Here we report for the first time that incorporation of bismuth (Bi) single atoms on defective CuO could significantly enhance the ECR reaction to C 2 H 4 by decreasing C–C coupling barriers. The overpotential for C 2 H 4 production is lowered by at least 50 mV, along with a two-fold improvement in the faradaic efficiency, reaching 60% at 400 mA cm −2 . The high performance is maintained even after 20 h of consecutive electrolysis. Control experiments along with density functional theory calculations suggest that the joint incorporation of Bi and oxygen vacancies greatly promotes CO 2 adsorption and lowers C–C coupling energy barriers, thereby improving the C 2 H 4 selectivity.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2020
·Vol. 22
·期 20
·11508-11518
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IF 3.43
Jing Chen,Hanling Yang,Hongquan Fu,Hongyan He,Qiang Zeng,Xuehui Li
Electrochemical oxidation is a promising and effective method for lignin depolymerization owing to its selective oxidation capacity and environmental friendliness. Herein, the electrooxidation of non-phenolic alkyl aryl ether monomers and β-O-4 dimers was experimentally (by cyclic voltammetry, in situ spectroelectrochemistry, and gas chromatography-mass spectroscopy) and theoretically (by DFT calculations) explored in detail. Compared to the reported literature (T. Shiraishi, T. Takano, H. Kamitakahara and F. Nakatsubo, Holzforschung, 2012, 66(3), 303–309), 1-(4-ethoxyphenyl)ethanol showed a distinguishable oxidation pathway, where the resulting carbonyl product surprisingly underwent a bond cleavage on alkyl–aryl ether to ultimately produce a quinoid like compound. In contrast, β-O-4 dimers, like 2-phenoxy-1-phenethanol and 2-phenoxyacetophenone also demonstrated electrochemical oxidation induced by Cβ–O and Cα–Cβ bond cleavages. For the oxidation products, the presence of the Cα-hydroxyl group in dimers was the key to selectively generate aldehyde-containing species under mild electrochemical conditions, otherwise it produces alcohol-containing products following a different mechanism compared to the CαO containing dimers.
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PubMed
高影响因子
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2023
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IF 5.7
Gui Li,Jianjie Hao,Jiayan Li,Pengyu Dai,Bo Wang,Yuanqi Li,Yi Tan,Xueqiang Cao
This work firstly evaluated the effect of temperature on the preparation of SiC coating using Al 2 O 3 as catalyst by pack cementation (PC) method. SiC/ZrB 2 -SiC-Si (ZSS) and SiC/ZrB 2 -SiC-Al 2 O 3 (ZSA) coating were prepared on the surface of C/C composites by PC combined with atmospheric plasma spraying (APS). The objective of this work is to study the influence of Si and Al 2 O 3 additives for ablation performances of ZrB 2 -SiC coating. The coated samples were subjected to ablation test, and the phase composition and microstructure evolution were investigated. The results indicated that SiC/ZSA coating had better ablation resistance because phase transformation and growth of ZrO 2 grain was restrained by Al 2 O 3 .
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ran Wang,Zhiding Zheng,Zhuo Li,Xiaoxiang Xu
Photocatalytic C-C coupling is a green and sustainable route to produce value-added chemicals. However, the product selectivity is generally non-tunable and there is a lack of an in-depth understanding of the dependence of product selectivity on the band structure of the semiconductor photocatalyst. Here, Zn x Cd 1-x S solid solutions have been explored for photocatalytic C-C coupling using benzyl alcohol as a typical reactant. The conversion rate of benzyl alcohol and selectivity of C-C coupling products is inherently linked to the solid solution level of Zn x Cd 1-x S which can be readily tuned. An optimal solid solution level has been found at Zn 0.6 Cd 0.4 S (x = 0.6) which delivers a conversion rate of 91.61% and a selectivity of 98.83% for C-C coupling products. These findings not only deepen the understanding on factors that affect product selectivity but also justify the usefulness of solid solutions in tuning the C-C coupling reactions.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Pei-dong Wu,Lanyun Li,Hu Li,Zhen Fang
Sustainable upgrading of biomass to high-value chemicals is greatly dependent on catalytic C-C/C-O bond cleavage of high selectivity. Here, an oxidation-enhanced photoelectrochemical protocol was developed to be capable of breaking different types of C-C bonds for efficiently producing aromatic carboxylic acids (85.0–99.8% yields) from lignin. Ni local electronic state of the prepared F-Fe 2 O 3 -Co:NiO x H y with excellent durability could be modulated, and high-valence Ni(Ⅳ) reactive species played a key role in the oxidative C-C bond scission of various lignin models. In-situ characterization and control experiments indicated that photocatalytic radical and electrocatalytic interface facilitated C-H/O-H delocalization, contributing significantly to the enhanced oxidation process. In addition, quantum calculations elaborated that photo-excited holes and Ni(Ⅳ) are key reactive species for enhancive electrocatalytic cleavage of different C-C bonds in lignin to exclusively furnish aromatic carboxylic acids. This research provides a renewable funnel strategy for using solar energy to produce high-value mono-functional products from biomass.
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高影响因子
Science China-Chemistry
·
2025
·
IF 9.7
Kang Kai,Wang Qiuxiang,Huang Hongpu,Zhuang Xinxin,Cai Junlin,Wang Tao,Wang Xue,Xie Zhaoxiong,Xie Shuifen
Despite utilization of state-of-the-art Cu-based catalysts, achieving high selectivity and stability in multicarbon (C 2+ ) compounds production through electrocatalytic CO 2 reduction reaction (CO 2 RR) remains a critical and challenging objective. Here we employ lattice chlorine-doped Cu 2 O nanocubes (Cl d -Cu 2 O NCs) with well-defined {100} facets as a model catalyst to demonstrate that halogen doping can serve as a versatile and effective strategy for modulating surface charge distribution, thereby enhancing asymmetric C–C coupling toward high-selectivity C 2+ products in CO 2 RR. Compared to Cl-free Cu 2 O NCs, Cl d -Cu 2 O NCs exhibit a greatly enhanced C 2+ Faraday efficiency, i.e., ∼85% at −1.1 V (versus the reversible hydrogen electrode). Additionally, the Cl d -Cu 2 O NCs demonstrate significantly enhanced long-term durability, attributed to better preservation of the cubic morphology and more stable Cu δ + states. In-situ electrochemical studies reveal that Cl d -Cu 2 O NCs facilitate the formation of the key asymmetric *COH and *OCCOH intermediates, ultimately leading to higher C 2+ products. Density functional theory (DFT) calculations confirm that the introduced Cl-dopants disrupt the charge balance of the Cu 2 O(100) surface, enriching the Cl-adjacent Cu atoms with more electrons compared to those near O atoms. This unbalanced charge distribution significantly reduces the free energy of the rate-determining step for asymmetric C–C coupling from the *CO to *OCCOH on Cl-doped Cu 2 O (100) surface, requiring only 1.04 eV, in contrast to 1.50 eV on pristine Cu 2 O(100) surface. This study provides valuable insights into the surface charge modulation of Cu 2 O catalysts via halogen doping for enhancing asymmetric C–C coupling and C 2+ production in CO 2 RR.
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ACS Catalysis
·
2025
·
IF 13.1
Rui Zhai,Zhenyu Wang,Chang Huang,Chao Zeng,Mengyue Gu,Tianqi Wang,Fanqi Bu,Shaobin Wang,Jinying Zhang
Phosphorus has various crystallographic structures and variable phosphorus-derived structures, which have attracted much attention due to its unique properties. One-dimensional phosphorus structures with atomic substitution in the phosphorus lattice are extremely favored due to their high specific surface area and stable single-atom dispersion. The precise crystal structures and single atomic substitution positions are crucial factors to understand the mechanism of single-atom effects but remain a big challenge. Herein, single crystals composed of 1D zigzag linear phosphorus selenium chains (ZLP-Se) have been produced and characterized by SC-XRD to be P18.56Se1.44 with a space group of Pnma (CSD-2348033). The exact Se substitution positions were further ascertained by calculations of the whole thermodynamic stability phase diagram to have three types of substitution patterns (Se1/P1 mixed occupied positions with intervals of 3Se+2P, 1Se+4P, and 1Se+1P+1Se+2P). The selenium-rich crystal plane (-10-1) has been demonstrated to significantly enhance CO2 adsorption and C−C coupling to obtain ethylene (C2H4). A high photocatalytic CO2 reduction performance (18.0 μmol g−1 h−1, 97.0% electron selectivity for C2H4) has been achieved by the ZLP-Se with the Ag cocatalyst. The adsorption of CO2* and CO* was found to be much stronger on the Se-rich surface of ZLP-Se. The CO* intermediates were found to be energetically favored for protonation and subsequent asymmetrical C−C coupling to produce C2H4, with COCHO* intermediates detected by in situ DRIFTS. The electron was also demonstrated by in situ XPS to transfer from Se and Ag to P under Xe lamp irradiation, confirming the electronic localization effect of ZLP-Se to yield C2H4.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Xuan Qi,Jun-Hao Wang,Jiang Shao,Hao Dong,Chen Li,Ya-Wen Zhang
Efficient production of multi-carbon (C₂ ⁺ ) products via CO 2 electroreduction reaction (eCO 2 RR) requires precise modulation of water activation, but still less investigated. In this work, we synthesized series of rare earth hydroxide-modified copper-based catalysts (RE(OH) 3 /CuO) to enhance water activation at the heterogeneous interfaces. Electrochemical evaluation showed significantly increased Faradaic efficiency for C₂ ⁺ products (up to 77.2 % at 500 mA cm −2 ) for the Sm(OH) 3 /CuO catalyst, alongside suppressed hydrogen evolution reaction (HER). This is caused by the facilitated hydrogenation of critical *CO intermediates via hydrogen spillover from the abundant Sm(OH) 3 /CuO interfaces in efficiently dissociating water molecules, promoting asymmetric C–C coupling on the Cu surfaces derived from CuO during eCO 2 RR. Experimental findings combined with DFT calculations indicated the critical role of the asymmetric *CO–*CHO coupling pathway on copper surfaces. This strategy demonstrates that rational design of interface water engineering and activation for a copper-based heterogeneous catalyst effectively promotes multi-carbon product formation in eCO 2 RR.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2017
·Vol. 31
·期 12
·e3854
·
IF 2.319
Xiaojun Ma,Guanghui Lv,Xu Cheng,Weijian Li,Rui Sang,Yong Zhang,Qiantao Wang,Li Hai,Yong Wu
An environmentally friendly palladium(II) catalyst supported on cyclodextrin-modified h-BN was successfully prepared. The catalyst was characterized by FT-IR, SEM, TG, XRD and XPS, and the loading level of Pd in h-BN@β-CD@Pd(II) was measured to be 0.088 mmol g −1 by ICP. It exhibits excellent catalytic activity for the Suzuki and Heck reactions in water, and can be easily separated and consecutively reused for at least nine times. In addition, a series of pharmacologically interesting products were successfully synthesized using this catalyst to demonstrate its potential applications in pharmaceutical industries. Above all, this work opens up an interesting and attractive avenue for the use of cyclodextrin-functionalized h-BN as an efficient support for hydrophilic heterogeneous catalysts.
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INTERNATIONAL JOURNAL OF POLYMER ANALYSIS AND CHARACTERIZATION
·
2025
·
IF 1.6
Junxia Chai,Hongbo Mo,Chuan Wang,Fengjie He,Jufen Huang,Li Ran,Weigang Fan,Yuepeng Fan,Fan Lu
This study developed Fe3O4@SiO2–C = C-based magnetic molecularly imprinted polymers for selective ibuprofen removal and detection. The optimized synthesis using an ibuprofen (IBP)/(3-aminopropyl)triethoxysilane (APTES)/tetraethyl orthosilicate (TEOS) molar ratio of 1:6:18 achieved a high adsorption capacity of 68.18 mg·g−1 and an imprinting factor of 2.17. The adsorption process followed pseudo-second-order kinetics and the Freundlich isotherm model, indicating multilayer binding behavior. The material demonstrated excellent reusability with only 2.8% capacity loss after five cycles and good reproducibility with a relative standard deviation of 4.48%. In magnetic solid-phase extraction applications, the recovery rate reached 81.61% to 96.40% for real water samples with a detection limit of 0.09 μg·mL−1. The polymers showed selective recognition of ibuprofen over structural analogs due to synergistic π-π interactions and hydrogen bonding, thus offering an efficient strategy for remediating pharmaceutical pollutants in water.
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