ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Zhenyao Li,Wei Wei,Xuli Hu,Zhen Zhang,Yangshun Hu,Yushan Wu,Yao Wang,Junchen Xu,Mingyue Ding
While engineering lattice strain has been proven effective in enhancing the electrochemical CO 2 reduction performance of a catalyst, the correlation between strain effect and the intrinsic catalytic mechanism has remained elusive. Herein, a photolithography-inspired method is proposed to regulate Cu(111) lattice strain. By irradiating the photosensitive Cu(Acac) sol–gel, Acac chelate bond undergoes π→π * electronic transition, and the ring-closed Cu(Acac) decompose into the stabilized Cu(Acac) mesh which presents as nanospots embedded onto the surface of the Cu cluster. The photoinduced nanospots serve to exert compressive strain to the Cu(111) lattice in which the lattice distance is reduced by 5.7–11.4%. Herein, the catalyst with 11.4% lattice compression exhibits enhanced C 2 H 4 production capabilities, reaching a maximal Faradaic efficiency of 57.00%, and a high partial current density of 456.01 mA cm −2 . Theoretical calculations reveal that the compressed Cu(111) lattice exhibits reduced surface energies, leading to a significant drop in the C─C coupling reaction free energy from 1.16 eV over the pristine lattice, to 0.57 eV over the 10% compressed lattice. Additionally, the 10% compressed lattice facilitates spontaneous *O splitting immediately after OC─CHO coupling which leads to the generation of C 2 H 4 -favoring *CCH intermediate.
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高影响因子
Catalysts
·
2024
·Vol. 14
·期 11
·756
·
IF 3.8
Xuekai Shan,Guolin Zhang,Ying Zhang,Shuobo Zhang,Fang Guo,Qi Xu
Selective CO2hydrogenation faces significant technical challenges, although many efforts have been made in this regard. Herein, a Ni-doped In2O3catalyst supported by g-C3N4was prepared using the co-precipitation method, and its composition, morphology, specific surface area, and band gap were characterized using TEM, XPS, BET, XRD, CO2-TPD, H2-TPR, UV-Vis, etc. The catalytic hydrogenation reduction of CO2to produce methanol was tested. Under low-photothermal conditions (1.0 MPa), the hydrogenation of carbon dioxide to methanol is stable, effective, and highly selective, with a spatiotemporal yield of 86.0 gMeOHh−1kgcat−1, which is 30.9% higher than that of Ni-In2O3without g-C3N4loading under the same conditions.
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高影响因子
Journal of Energy Chemistry
·
2024
·
IF 14
Guan Wang,Shengtao Zhong,Xiaoqian Xiong,Jing Li,Fangyuan Wang,Li Huo,Daoxiong Wu,Xingqi Han,Zhitong Wang,Qi Chen,Xinlong Tian,Peilin Deng
Bismuth-based catalysts are highly promising for the electrochemical carbon dioxide reduction reaction (eCO 2 RR) to formate product. However, achieving high activity and selectivity towards formate and ensuring long-term stability remains challenging. This work reports the oxygen plasma inducing strategy to construct the abundant grain boundaries of Bi/BiO x on ultrathin two-dimensional Bi nanosheets. The oxygen plasma-treated Bi nanosheet (OP-Bi) exhibits over 90% Faradaic efficiency (FE) for formate at a wide potential range from −0.5 to −1.1 V, and maintains a great stability catalytic performance without significant decay over 30 h in flow cell. Moreover, membrane electrode assembly (MEA) device with OP-Bi as catalyst sustains the robust current density of 100 mA cm −2 over 50 h, maintaining a formate FE above 90%. In addition, rechargeable Zn-CO 2 battery presents the peak power density of 1.22 mW cm −2 with OP-Bi as bifunctional catalyst. The mechanism experiments demonstrate that the high-density grain boundaries of OP-Bi provide more exposed active sites, faster electron transfer capacity, and the stronger intrinsic activity of Bi atoms. In situ spectroscopy and theoretical calculations further elucidate that the unsaturated Bi coordination atoms between the grain boundaries can effectively activate CO 2 molecules through elongating the C–O bond, and reducing the formation energy barrier of the key intermediate (*OCOH), thereby enhancing the catalytic performance of eCO 2 RR to formate product.
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Plasma Processes and Polymers
·
2024
·Vol. 21
·期 7
·2400037
·
IF 2.9
Xuming Zhang,Yun Shan,Zhi Sun,Hua Pan,Yuzhen Jin,Zuchao Zhu,Liancheng Zhang,Wenhao Lin,Zhengbo Dai,Zhengang Lou,Huaming Li,Kai Li
Plasma catalytic CO 2 hydrogenation to methanol over MnO x /ZrO 2 catalyst was investigated in this work. A boosted methanol yield of 4.6 mg/h was obtained over MnO x /ZrO 2 catalyst, while it was only 0.0 and 0.7 mg/h for ZrO 2 and MnO x catalyst, respectively. The interaction between MnO x and ZrO 2 was responsible for the enhanced methanol yield. It resulted in sufficient oxygen vacancy. The in situ DRIFT spectra was conducted to reveal the plasma catalytic CO 2 hydrogenation to methanol reaction mechanism and the key intermediates of HCOO and CH 3 O species were determined. The sufficient oxygen vacancy promoted the formation of the key intermediates, especially the CH 3 O species.
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高影响因子
JOURNAL OF POLYMER RESEARCH
·
2025
·Vol. 32
·期 3
·1-9
·
IF 2.8
Xian Wenqi,He Maoyi,Zheng Rui,Liu Zhu,Lu Ming,Chu Yuehuan,Cao Hao
CO 2 copolymer diol (PPCD) with superior transparency is an indispensable raw material for the polyurethane, especially for waterborne polyurethane coatings. However, commercial PPCD is generally opaque. In this work, A sustainable, colorless and transparent PPCD was prepared by using carbon dioxide (CO 2 ) and propylene oxide (PO) as raw materials. Research shows that the increase in CO 2 content (from 23.5 wt.% to 31.5 wt.%) will affect the transparency and thermal stability of PPCD and the transparency of PPCD with 29.1 wt.% CO 2 content is even higher than 90%, while the 5 wt.% mass loss temperature reaches 240.1 ℃. Furthermore, a series of waterborne polyurethane (WPU) was successfully synthesized by prepolymer method with PPCD as the soft segment. With the increase of CO 2 content, the thermodynamic property of WPU was significantly improved. When CO 2 content increased from 23.50 wt.% to 31.50 wt.%, the tensile strength increased from 23.27 MPa to 34.63 MPa and the elongation at break decreased from 750.85% to 520.37%, accompanied by the glass-transition temperature increased from -49.7 ℃ to -34.5 ℃. In addition, it was found that WPU prepared by transparent PPCD has better tensile strength, transparency, and storage stability. A new inspiration was provided for its application in the fields of optical components, transparent medical materials and UV curable coatings.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Xi Liu,Delong Hou,Demeng Liu,Siyu Pan,Jun Yan,Qi Zeng,Yi Chen
The α-methyl esterification of natural fatty acid methyl esters (FAMEs) is an essential approach for preparing high-value chemicals such as migration-resistant bioplasticizers, polyester precursors, and anionic surfactants. However, previous strategies are primarily based on time-consuming Claisen condensation, which utilizes petroleum-derived dimethyl carbonate (DMC) as a building block for α-methyl esterification, as well as a NaH/DMF deprotonation system with a highly explosive risk. Here, we present an efficient approach that harnesses carbon dioxide as a green C1 building block to facilitate rapid, nonexplosive α-methyl esterification of FAMEs, producing fatty acid dimethyl esters with high yield (>85%) at ambient temperature within 3 h. Various natural FAMEs, even those derived from waste cooking oil, are amenable to this approach. Our findings establish a robust strategy for α-methyl esterification of FAMEs, bringing the production of high-value chemicals from FAMEs one step closer to sustainability.
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高影响因子
ADVANCED MATERIALS
·
2025
·Vol. 37
·期 39
·2510192
·
IF 26.8
Haozhou Yang,Na Guo,Shibo Xi,Haiyuan Zou,Jiayi Chen,Lei Fan,Yukun Xiao,Qian He,Lele Duan,Pengfei Wei,Guoxiong Wang,Chun Zhang,Lei Wang
Carbon nanotubes (CNTs) are widely used as supports for immobilizing molecular electrocatalysts, such as for CO 2 reduction (CO 2 R), with π-π interactions often assumed to govern the catalyst immobilization. However, the nature of catalyst/CNTs interactions remains insufficiently understood. Here, nickel phthalocyanine (NiPc) is investigated, a benchmark CO 2 R catalyst, supported on CNTs. NiPc preferentially anchors at defect-sites on CNTs rather than adsorbing uniformly via π-π stacking is found, an observation validated by theoretical simulations. Notably, CNTs with the fewest defects, despite exhibiting non-uniform NiPc distribution, deliver the highest CO 2 R activity and CO selectivity. Operando X-ray absorption spectroscopy reveals that high defect densities induce D 4 h symmetry distortion of the NiPc macrocycle under cathodic bias, compromising catalyst integrity and CO 2 R performance. Guided by these insights, CNT defect density is optimized via thermal graphitization, yielding a NiPc/CNT composite with unprecedented selectivity (CO:H 2 > 16 100:1) and a turnover frequency of 1072 s⁻ 1 at −0.60 V versus RHE, switching off the competing hydrogen formation. Integrated into a 100 cm 2 zero-gap electrolyzer, the optimized catalyst sustains 50 A current with >95% CO selectivity at ≈3.5 V, outperforming state-of-the-art Ag-based systems. This work establishes CNT defect-engineering as an effective strategy for advancing molecular catalysts for CO 2 R electrolysis.
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PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Zhihe Zhang,Zihang Yu,Kai Feng,Binhang Yan
CO 2 methanation is gaining renewed attention due to the emerging application needs such as the power-to-gas concept and long-term space exploration missions. Maximizing the amounts of interfacial sites generally regarded as the efficient active sites is considered to be one of the most direct means to enhance catalytic activity but few breakthroughs have been made. Here, Eu 3+ is introduced to Ni/CeO 2 to promote the Ni-CeO 2 interaction, resulting in a remarkable low-temperature CO 2 methanation activity. Structural characterization indicates that the Ni/CeEu(9:1) catalyst achieves higher Ni dispersion compared to Ni/CeO 2 , which consequently generates more interfacial sites. More interfacial sites enhance the proportions of bidentate carbonates closer to interfacial sites as a faster hydrogenated species during the catalytic process, leading to enhanced low-temperature CO 2 methanation activity over the Ni/CeEu(9:1) catalyst. This work provides a chemical strategy to enhance the amounts of active sites and bring insights into the origin of enhanced catalytic performance.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Zheyang Liu,Jianli Liang,Qianqian Song,Yang Li,Zhiquan Zhang,Min Zhou,Wei Wei,Hui Xu,Chun-Sing Lee,Huaming Li,Zhifeng Jiang
Efficient conversion of CO 2 to high value-added chemical products is a promising strategy for achieving carbon neutrality . Although the photocatalyst technique has been made widespread researched, highly efficient photoreduction CO 2 with metal-free photocatalysts remains a challenge. Herein, we report a zero-dimensional black phosphorus quantum dots (BPQDs)-decorated one-dimensional carbon nitride nanotubes (CNNT) photocatalyst that reduces CO 2 to CO with a rate of 44.6 μmol g –1 h –1 , which is better than the similar photocatalysts and pristine carbon nitride nanotubes . Synchrotron radiation XAFS measurements substantiate the construction of N-P electron transfer channels within BPQDs and CNNT. Time-resolved PL spectrum demonstrates the faster separated electron hole pairs . In situ irradiated X-ray photoelectron spectroscopy confirms the photogenerated-electron flow trend and the active site of photocatalytic reaction. Moreover, the main intermediate *COOH is verified by in situ FT-IR characterization which is corresponding to the previous research. The construction of atomic-level N-P charge transfer channel efficiently facilitates the charge transfer and accelerates the catalytic rate. This work provides a novel insight into the design of BPQDs-anchoring heterostructures for photocatalytic CO 2 reduction.
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高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Tophet Wongladprom,Qi Li,Tianyu Guo,Hui Wu,Jie Li,Gang Wang,Chunshan Li
A highly effective catalyst is desired for CO 2 selective hydrogenation to methanol due to the kinetic limitation of this process, considering the heavy impact of CO 2 emission on global environment. Herein, a type of ammonization-treated CuMo catalyst was developed for CO 2 -to-methanol hydrogenation, which contains MoN and Mo 2 N species. The effect of catalyst preparation conditions on the physicochemical properties of the resulting sample was systematically investigated using multiple characterization techniques, including physical N 2 adsorption and desorption isotherms, XRD, HRTEM, XPS, Cu Auger spectra, H 2 -TPR and CO 2 -TPD. Structure-activity relationships analysis revealed that the proportion of Cu 0 and Mo δ+ (1 < δ < 4) in the catalyst is linearly correlated to the CO 2 transformative rate and methanol selectivity, respectively, which is considered to show synergistic effect on methanol production. Consequentially, the methanol production could reach up to 177.2 mg/g cat /h with a selectivity of 95.7 % at 230 °C and 4 MPa. In addition, the catalytic mechanism exploration employing in situ IR indicated the CO 2 hydrogenation towards methanol follows the formate route, and the Mo δ+ species facilitated the stabilization of CO 2 -derived reactive intermediates on the catalyst surface. Additionally, kinetic studies reveal methanol formation is primarily limited by CO 2 adsorption/activation rather than H 2 dissociation.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2016
·
IF 2.567
Zeguang Yin,Ke Wang,Pengfei Zhao,Xiaoli Tang
The water hydration and subsequent calcination (denoted as hydration–calcination) technique was used to modify the microstructure of lithium orthosilicate (Li4SiO4) prepared by solid-state reactions. The original and modified Li4SiO4 sorbents were characterized by X-ray diffraction, Fourier transform infrared spectroscopy, nitrogen adsorption, scanning electron microscopy, and thermogravimetric analysis. The cyclic capacity of these sorbents was further examined using a dual fixed-bed reactor. After treatment by water hydration, most of the Li4SiO4 transformed into LiOH and Li2SiO3. Moreover, following subsequent calcination, the sample exhibited a looser structure with a smaller particle size compared with the original Li4SiO4. This favorable structure was responsible for improved CO2 chemisorption properties, as measured by a higher capacity, faster absorption kinetics, and improved stability.
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高影响因子
Journal of Materials Chemistry A
·
2012
·Vol. 1
·期 3
·752-758
·
IF 0
Heping Ma,Hao Ren,Xiaoqin Zou,Fuxing Sun,Zhuojun Yan,Kun Cai,Dayang Wang,Guangshan Zhu
Novel porous aromatic frameworks, PAF-18-OH and its lithiated derivative PAF-18-OLi, have been successfully synthesized. In particular, PAF-18-OLi displays significant enhancement of H2 and CO2 adsorption capacity, especially for CO2 uptake (14.4 wt%). More valuably, the stable PAF-18-OLi material exhibits high CO2/N2 selectivity, as high as 129 in the case of CO2 capture from simulated post-combustion flue gas mixtures (85% N2 and 15% CO2). Furthermore, the PAF-18-OLi has shown improved H2 storage capacity after lithiation.
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