ACS Catalysis
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2024
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IF 11.3
Weijie Geng,Di Zhang,Ni Zhen,Jianxin Du,Jing Dong,Chengpeng Liu,Shi-Lu Chen,Yingnan Chi,Changwen Hu
The electrochemical coupling of biomass platform molecules to biofuels provides a promising method for addressing energy crises and environmental issues. However, achieving high yields of C–C coupling products under ambient conditions remains a challenge. Herein, we present a highly efficient electrocatalyst, [Cu(pz)]3[PW12O40] (Cu-PW12), fabricated by combining a Cu-pz complex (pz = pyrazine), a redox catalytic center, with Keggin-type PW12O40, and an electron sponge. Cu-PW12 exhibits remarkable catalytic activity for the electroreductive C–C coupling of furfural (FF), a bulk and low-cost biomass platform chemical, to produce a jet fuel precursor, hydrofuroin (HDF). Under neutral and ambient conditions, over 99% of FF is converted and the selectivity of HDF reaches 91.2%. Furthermore, experimental and theoretical studies, including control experiments, kinetic isotope studies, electrochemical and spectral analyses, and DFT calculations, reveal a synergistic catalysis effect between Cu center and PW12. The introduction of PW12 not only facilitates electron transfer, improving FF conversion, but also changes the rate-determining step, favoring the formation of HDF. Under turnover conditions, the Cu-PW12 catalyst is initially reduced and then FF is reduced by the Cu center to ketyl radical after protonation on the electrode surface. Finally, the self-coupling of two ketyl radicals in solution leads to the generation of HDF.
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Journal of Energy Chemistry
·
2024
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IF 14
Xiaoyue Zhang,Yong Yang,Yingjie Hu,Lijun Xiong,Tianyu Wang,Panjie Li,Jinyou Shen
Photothermal catalytic CO 2 conversion provides an effective solution targeting carbon neutrality by synergistic utilization of photon and heat. However, the C–C coupling initiated by photothermal catalysis is still a big challenge. Herein, a three-dimensional (3D) hierarchical W 18 O 49 /WTe 2 hollow nanosphere is constructed through in-situ embodying of oxygen vacancy and tellurium on the scaffold of WO 3 . The light absorption towards near-infrared spectral region and CO 2 adsorption are enhanced by the formation of half-metal WTe 2 and the unique hierarchical hollow architecture. Combining with the generation of oxygen vacancy with strengthened CO 2 capture, the photothermal effect on the samples can be sufficiently exploited for activating the CO 2 molecules. In particular, the close contact between W 18 O 49 and WTe 2 largely promotes the photoinduced charge separation and mass transfer, and thus the *CHO intermediate formation and fixedness are facilitated. As a result, the C–C coupling can be evoked between tungsten and tellurium atoms on WTe 2 . The ethylene production by optimized W 18 O 49 /WTe 2 reaches 147.6 μmol g − 1 with the selectivity of 80%. The in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and density functional theory (DFT) calculations are performed to unveil the presence and significance of aldehyde intermediate groups in C–C coupling. The half-metallic WTe 2 cocatalyst proposes a new approach for efficient CO 2 conversion with solar energy, and may especially create a new platform for the generation of multi-carbon products.
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Journal of Energy Chemistry
·
2024
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IF 14
Hongqiang Yang,Jianfeng Zheng,Guoyu Wang,Yifei Gao,Yatao Yang,Jia Li,Xiaojin Han,Yan Cui,Zhanggen Huang
Photoelectrocatalytic coupling CO 2 and volatile organic compounds (VOCs) is a promising green strategy for the synergistic conversion of the two carbon-containing resources to C 2 products. The catalytic efficiency is always at the mercy of chemical inertness of CO 2 and the competitive hydrogen evolution of H 2 O. Herein, a modified g-C 3 N 4 /ZnAl-LDH Z-scheme heterojunction catalyst with dual reaction site was rationally designed and precisely constructed. The Faraday efficiency of ethanol reached 68.67% with a corresponding formation rate of 227.3 μmol g −1 h −1 . As revealed by in-situ characterizations and density functional theory calculations, CO 2 and HCHO were absorbed at Zn site and N site, respectively. Then, *CO generated from CO 2 and HCHO was converted to *CH 3 O and *CHO on the dual-active-site heterojunction. The detailed reaction mechanism experiments indicated that C–C coupling only occurred between *CO and *CH 3 O in electrocatalysis process. Apart from the “*CO + *CH 3 O” path, another “*CO + *CHO” coupling path was also detected in photoelectrocatalytic process. The selectivity of ethanol was significantly enhanced due to the synthesis of dual-site catalyst and the dual-path coupling path between CO 2 and HCHO simultaneously driven by light and electricity.
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CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Su Wang,Qifang Sun,Chen Li,Dongge Wang,Yue Ma,Hongzhou Zhang,Xixi Shi,Lianqi Zhang,Dawei Song
Given the high combustion or explosion potential of liquid electrolyte, polymer electrolytes have attracted intensive attention due to high safety, compatible interface and flexible processability. However, the related low ionic mobility remains an issue for related wide application. Herein, a crosslinked polymer electrolyte (abbreviated as PMEP) comprising abundant oxygen-contained groups (C-O-C/C=O) is developed. With the crosslinking agent of ethoxylated trimethylolpropane triacrylate (ETPTA), a high transference number ( t Li + =0.69) is obtained since C-O/C=O are conducive to the transfer of Li ions. Specifically, C=O group exists in individual monomers in order to be applicable to high voltage cathode, therefore, a criss-cross network containing abundant sites conducive to ion transport is constructed and rapid ion transfer as well as enhanced mechanical strength can be realized even in high potential system. With the coordination effect of C-O and C=O, PMEP exhibits rapid Li ion transfer and a wide electrochemical stability window of 5.1 V. As for Li//Li symmetrical cell, a stable voltage profile with slight polarization of 60 mV is displayed for over 550 h at 1 mA cm −2 . After assembled with LiNi 0.8 Co 0.15 Al 0.05 O 2 cathode, a high discharge specific capacity of 190.6 mAh g −1 is delivered and the capacity retention reaches 86 % at 0.1C for 100 cycles. This work provides a promising method for designing high-performance polymer electrolytes for lithium metal batteries.
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BIOMASS & BIOENERGY
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2025
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IF 5.8
Shanshan Shao,Haochuan Yang,Yu Cao,Jiayuan Sun,Xiaohua Li,Shiliang Wu
This study aims to produce oxygen-containing precursors for jet fuel through directed carbonylation and C-C coupling of aqueous bio-oil (AQBO), focusing on exploring the impact of the complex compositions in AQBO and the catalyst properties on reaction mechanisms in the preparation process. There are two major limitations among current research on the preparation of jet fuel precursors from biomass: first, most studies are based on model compounds of AQBO; second, the yield of jet fuel precursors is low. In this study, to address these limitations, the mechanisms of carbonylation and C-C coupling were investigated by mixing model compounds (furfural, acetone and butyraldehyde) in AQBO, and the relative peak area of the jet fuel precursor reached 89.6 % when 16 % furfural was mixed. The priority of the coupling reaction of aldehydes and ketones was described as follows: cycloketone with linear aldehyde > cycloketone with cycloketone > cycloketone with linear ketone. Based on the investigation of active sites in the composite catalyst for carbonylation and coupling reactions, we designed an improved catalyst using red mud (RM) as a bifunctional catalyst carrier. The efficient conversion of agricultural wastes and red mud into jet fuel is achieved, with the resulting products further serving as sustainable aviation fuel (SAF) precursors, demonstrating potential for carbon intensity (CI) reduction and facilitating the valorization of low-value biomass and industrial residues.
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APPLIED ORGANOMETALLIC CHEMISTRY
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2017
·Vol. 31
·期 12
·e3854
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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.
研究领域:
材料科学
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催化化学
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APPLIED CATALYSIS B-ENVIRONMENTAL
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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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INTERNATIONAL JOURNAL OF POLYMER ANALYSIS AND CHARACTERIZATION
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2025
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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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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2025
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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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Science China-Chemistry
·
2025
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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.
研究领域:
电催化
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材料科学
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环境化学
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纳米技术
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物理化学
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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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.
研究领域:
电催化
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能量转换
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材料科学
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环境化学
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二氧化碳还原
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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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