Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 42
·23817-23827
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IF 12.732
Manman Feng,Xuemei Wu,Huiyuan Cheng,Zihao Fan,Xiangcun Li,Fujun Cui,Shuai Fan,Yan Dai,Guangping Lei,Gaohong He
The diatomic catalysts (DACs) provide a new strategy for efficient catalysis of CO2 reduction reaction (CO2RR) owing to their maximum atomic utility and more flexible active sites. However, it is still challenging to precisely design heteronuclear diatomic active centers and understand the coordination mechanism of binary sites at the atomic level. Herein, a nitrogen-doped carbon matrix with precisely controlled Fe–Cu diatom sites is synthesized through a metal–organic framework. The as-obtained Fe/Cu–N–C catalyst exhibits an excellent CO faradaic efficiency (>95% over a wide potential range of −0.4 to −1.1 V vs. RHE, 99.2% at −0.8 V vs. RHE), a high turnover frequency (5047 h−1 at −1.1 V vs. RHE), and a low overpotential (50 mV), thus outperforming most reported atomically dispersed catalysts. Further density functional theory calculations indicate that the synergy between Fe–Cu diatoms causes rapid charge transfer and effectively adjusts the position of the d-band center, which reduces the energy barriers for *COOH formation and *CO desorption. This work provides a new approach for advancing universal synthesis strategies to construct heteronuclear diatomic catalysts and explore synergistic effects.
研究领域:
材料科学
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催化化学
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能源转换
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DOI
高影响因子
RSC Advances
·
2024
·Vol. 14
·期 29
·21151-21157
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IF 3.9
Jianwei Yang,Xianghao Han,Xiao Feng
As an emerging category of crystalline porous materials, covalent organic frameworks (COFs) are primarily synthesized via solvothermal methods. However, achieving rapid synthesis of COFs through this approach poses a significant challenge. To address the issue of slow synthesis, we studied the crystallization process of aminal-linked COFs via the condensation of a cost-effective aldehyde and secondary amine, and successfully expedited the synthesis of COFs within a one-hour duration. Furthermore, gram-scale aminal-linked COFs with abundant ultra-microporous channels demonstrated promising potential for CO2/CH4 separation. This study enables the rapid synthesis of aminal-linked COFs from cheap raw materials, which lays a foundation for their practical applications.
研究领域:
材料科学
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化学工程
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DOI
PubMed
高影响因子
JOURNAL OF POLYMER RESEARCH
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2025
·Vol. 32
·期 3
·1-9
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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.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
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2025
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IF 4.3
Yadong Du,Xiangtong Meng,Jun Qi,Benxiang Gong,Yangjun Ma,Jiachun Li,Hongqi Zou,Jieshan Qiu
Electrochemical CO 2 reduction (ECR) to value-added products provides a pathway to reduce CO 2 emission and to enable a closed carbon cycle. Compared to powdered catalysts, self-supporting electrocatalysts have more prominent advantages such as high charge transfer capacity and the ability to serve directly as working electrodes without the need for binders. Herein, a self-supporting catalyst featuring SnO 2 nanoparticles incorporated into porous carbon nanofiber (SnO 2 -PCNF) was crafted via electrospinning followed by annealing in CO 2 . SnO 2 -PCNF can directly function as working electrode for ECR to produce HCOOH, achieving a high Faradaic efficiency of 92.3%. Also, the SnO 2 -PCNF can stably catalyze ECR process for more than 50 h. Theoretical calculations and in-situ Raman spectroscopy elucidate the underlying ECR mechanism over SnO 2 -PCNF, wherein the catalyst significantly reduces the energy barrier of the rate-determining step. This effectively suppresses the competitive hydrogen generation. This work provides some insights into design of binder-free and high-performance ECR electrocatalysts.
研究领域:
材料科学
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环境科学
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能源化学
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产品关联
DOI
高影响因子
CHEMOSPHERE
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2020
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IF 5.778
Dong Xia,Ange Maurice,Antoine Leybros,Jong-Min Lee,Agnes Grandjean,Jean-Christophe P. Gabriel
Removal of brominated flame retardants (BFRs) from polymers before disposal or recycling will alleviate negative environmental effects and ensure safe usage of recycled products. Extraction of BFRs in supercritical CO 2 is appealing but also presents challenges to industries due to limited solubility and lack of kinetic studies. For a more comprehensive evaluation of supercritical extraction potentialities, we (i) developed an on-line pressure apparatus that is compatible with both the FTIR and UV–vis spectrometers to enable kinetic and thermodynamic studies; (ii) studied kinetic extraction involving three conventional and two novel BFRs as well as three typical polymeric matrix. Solubilities were determined using the gravimetric method or X-ray fluorescence. FTIR exhibited a superior applicability compared to UV–vis in the following BFR extraction’s time-dependency binary and ternary systems . We observed that faster stirring speed, higher temperature, and finer particle size can accelerate the overall extraction kinetics. In binary systems, it took less than 2 h to achieve equilibrium for each BFR at 60 °C, 25 MPa and 1000 rpm. In the presence of polymeric matrix, slower extraction kinetics were observed due to the occurrence of competitive dissolution and molecular diffusion within the matrix. Mathematical models derived from irreversible desorption and Fick’s diffusion laws fitted well with the observed extraction kinetics of BFRs, thus enabling us to identify the rate-determining step. The high solubilization rate coefficients that we measured for BFRs revealed that the dynamic extraction process in up-scaling design could compensate for the low solubility with flowing supercritical CO 2 .
研究领域:
环境科学
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化学工程
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DOI
高影响因子
MOLECULES
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2024
·Vol. 29
·期 14
·3334
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IF 4.2
Aizhen Liao,Zhengchu Liu,Yiqing Wei,Qinghua Xie,Ting Kong,Maolin Zeng,Wenpeng Wang,Chao Yang,Linji Zhang,Yonggang Xu,Yong Zhou,Zhigang Zou
The synthesis of the accurate composition and morphological/structural design of multielement semiconductor materials is considered an effective strategy for obtaining high-performance hybrid photocatalysts. Herein, sulfur vacancy (Vs)-bearing In2S3/CuInS2microflower heterojunctions (denoted Vs-In2S3/CuInS2) were formed in situ using In2S3microsphere template-directed synthesis and a metal ion exchange-mediated growth strategy. Photocatalysts with flower-like microspheres can be obtained using hydrothermally synthesized In2S3microspheres as a template, followed by Ostwald ripening growth during the metal cation exchange of Cu+and In3+. The optimal heterostructured Vs-In2S3/CuInS2microflowers exhibited CO and CH4evolution rates of 80.3 and 11.8 μmol g−1h−1, respectively, under visible-light irradiation; these values are approximately 4 and 6.8 times higher than those reported for pristine In2S3, respectively. The enhanced photocatalytic performance of the Vs-In2S3/CuInS2catalysts could be attributed to the synergistic effects of the following factors: (i) the constructed heterojunctions accelerate charge-carrier separation; (ii) the flower-like microspheres exhibit highly uniform morphologies and compositions, which enhance electron transport and light harvesting; and (iii) the vs. may trap excited electrons and, thus, inhibit charge-carrier recombination. This study not only confirms the feasibility of the design of heterostructures on demand, but also presents a simple and efficient strategy to engineer metal sulfide photocatalysts with enhanced photocatalytic performance.
研究领域:
材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Surfaces and Interfaces
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2025
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IF 6.3
Chaoqiang Li,Xiangyu Xu,Aizhong Jia
Photocatalytic reduction of CO 2 to chemical fuels is a promising strategy to alleviate the greenhouse effect and energy crisis. This article successfully fabricated Ag/CdS composites with ohmic junction using a two-step method and further verified them by DFT calculations. Meanwhile, photoelectrochemical and electron paramagnetic resonance tests show that Ag/CdS has higher photocurrent density and lower charge transfer resistance, suggesting that the ohmic junction achieves ultrafast electron transfer from CdS to Ag under light irradiation, significantly promoting the separation of photogenerated carriers. Furthermore, the localized plasmon resonance (LSPR) of Ag enhances the light absorption of the catalyst and generates a large number of hot electrons for the photocatalytic reduction reaction. The synergistic effect of ohmic junction and LSPR gives high electron density at the reaction site, which promotes the multiple proton-coupled electron reactions leading to highly selective photoconversion of CO 2 to CH 4 . Under the optimized conditions, the CH 4 yield of the synthesized Ag/CdS is 68.6 μmol·g −1 ·h −1 , which is 25.4 times higher than that of bare CdS, and the CH 4 selectivity increases from 53.8% to 90.1%. This study provides a new idea for the design of CdS-based materials for highly selective reduction of CO 2 to CH 4 .
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2022
·Vol. 12
·期 15
·4817-4825
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IF 6.177
Shilin Kang,Zhijun Li,Zhikun Xu,Ziqing Zhang,Jianhui Sun,Ji Bian,Linlu Bai,Yang Qu,Liqiang Jing
Although g-C3N4-based heterojunctions show promise for photocatalytic CO2 reduction, enhancing charge separation and creating sufficient catalytic sites remain challenges. In this study, mixed-valence CuPc/graphene/g-C3N4 (HT-CuPc/G/UCN) ultrathin heterojunctions (∼4.8 nm thickness) with Cu1+/Cu2+ species were constructed by H-bond induced assembly and subsequent post-treatment with H2. The optimized H100-CuPc/G/UCN sample showed 36-times higher activity than bare ultrathin g-C3N4 (UCN) for photocatalytic CO2 reduction to CO. Based on atomic force microscopy images, normalized photocurrent action spectra, electron paramagnetic resonances, and in situ diffuse reflectance infrared Fourier transform spectra, it was confirmed that the unexpected photocatalytic activity of H100-CuPc/G/UCN was attributed to the dual-functional roles of the introduced graphene: to increase the optimized amount of CuPc and enhance the high-level-energy electrons transferring from UCN to CuPc and the created Cu1+/Cu2+ species by H2 reduction as active catalytic sites for CO2 reduction. This work provides a comprehensively feasible strategy for preparing rational heterojunctions toward high-efficiency solar-driven CO2 reduction.
研究领域:
材料科学
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环境科学
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化学
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DOI
高影响因子
ENERGY
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2024
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IF 9
Fanli Meng,Kun Fu,Xueli Wang,Bonan Ye,Pan Zhang,Lemeng Wang,Dong Fu
Previous work has shown that non-aqueous absorbent composed of dimethyl sulfoxide (DMSO) and 2-ethylhexylan-1-amine (EHA) is superior to commercial monoethanolamine (MEA) in both absorption of CO 2 and desorption. However, the price of DMSO is too high, which leads to the high cost of reagents. It is worthwhile to choose a cheap solvent instead of DMSO, which can also achieve satisfactory absorption and desorption performance. Around this goal, we selected diethylene glycol diethyl ether (DEGDEE) to form a non-aqueous absorbent with EHA and investigated the absorption and desorption performance. The desorption efficiency of 70 wt% EHA +30 wt% DEGDEE was 99 % at 373 K. The desorption efficiency was 89.4 %, and the desorption energy consumption was only 45.1 % of MEA when the water content was 10 wt%. DEGDEE can achieve similar or even better performance than DMSO, while the cost of DEGDEE (12000–31000 RMB/ton, technical grade purity 99 %) is lower than DMSO (40000–48000 RMB/ton, technical grade purity 99 %). In addition, it also has a good recycling capacity. These advantages will certainly endow this newly developed absorbent with great application prospects in the field of CO 2 capture.
研究领域:
化学工程
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环境科学
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材料科学
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产品关联
DOI
高影响因子
RARE METALS
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2025
·
IF 11
Wang Dan-Dan,Xu Meng-Yang,Lin Zhao-Xin,Wu Jia-Hui,Yang Wei-Ting,Li Hong-Ji,Su Zhong-Min
The goal of photocatalytic CO 2 reduction is to obtain a single energy-bearing product with high efficiency and stability. Consequently, constructing highly selective photocatalysts with enhanced surface and optoelectronic properties is crucial for achieving this objective. Here, we have developed a simple one-pot vulcanization method to synthesize a MIL-68(In)-derived CdIn 2 S 4 /In 2 S 3 heterojunction that exhibited stable and high selectivity. Multiple characterizations of the CdIn 2 S 4 /In 2 S 3 heterojunction revealed a hierarchical tubular structure with numerous surface reactive sites, a high visible-light utilization rate ( λ < 600 nm), efficient charge separation, and a prolonged charge-carrier lifetime. Moreover, an S-scheme charge transfer mechanism, based on the interleaved band between the two components, improved the reduction capability of the electrons. Benefiting from the compositional and structural synergy, the yield CO by CdIn 2 S 4 /In 2 S 3 -250 (CI-250) reached 135.62 μmol·g −1 ·h −1 , which was 49.32 times and 32.88 times higher than that of In 2 S 3 and CdIn 2 S 4 , respectively. The CdIn 2 S 4 /In 2 S 3 heterojunction exhibited a quantum efficiency of 4.23% with a CO selectivity of 71%. Four cycle tests confirmed the good stability and recyclability of the CI-250. This work provides a new approach for designing and preparing high-performance hollow MOFs-based photocatalysts for scalable and sustainable CO 2 reduction.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
RSC Advances
·
2024
·Vol. 14
·期 20
·13719-13733
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IF 3.9
Qilin Han,Zhiyao Wu,Yu Zhou,Yongxin Lei,Bingying Nie,Leilei Yang,Wenbin Zhong,Nannan Wang,Yanqiu Zhu
Developing low-cost and efficient photocatalyst/co-catalyst systems that promote CO2 reduction remains a challenge. In this work, Ag–Ti3C2Tx composites were made using a self-reduction technique, and unique Ag–Ti3C2Tx/ZnO ternary heterojunction structure photocatalysts were created using an electrostatic self-assembly process. The photocatalyst's close-contact heterogeneous interface increases photogenerated carrier migration efficiency. The combination of Ti3C2Tx and Ag improves the adsorption active sites and reaction centers for ZnO, making it a key site for CO2 adsorption and activation. The best photocatalysts had CO and CH4 reduction efficiencies of 11.985 and 0.768 μmol g−1 h−1, respectively. The CO2 conversion was 3.35 times better than that of pure ZnO, which demonstrated remarkable stability even after four cycle trials with no sacrificial agent. Furthermore, in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS) and valence band spectroscopy were utilized to propose the photocatalytic reaction mechanism and electron transfer channels of the Ag–Ti3C2Tx/ZnO system, confirming that CHO* and CO* are the important intermediates in the generation of CH4 and CO. This study introduces a novel method for the development of new and efficient photocatalysts and reveals that Ti3C2Tx MXene is a viable co-catalyst for applications.
研究领域:
材料科学
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环境科学
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化学
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Xinyu Sun,Quanqi Zhang,Sihan Li,Yiming Zhang,Meiyu Liu,Binbin He,Yi Mei,Yun Zu
Ca-FAU zeolite sorbents have been recognized as one of promising CO 2 capture materials, while it is subject to the change in the speciations and locations of Ca 2+ species as adsorption sites in the FAU zeolite due to its susceptible migration. In this paper, a facile strategy is reported by tuning calcination temperatures and Ca loadings, to maximize the utilization of Ca 2+ species in the supercages of CaNaX zeolites. Detail characterizations of TG-MS, in situ FTIR spectroscopy and XRD Rietveld refinement reveal the changeable regular in the chemical speciations, locations and number of Ca 2+ species in the CaNaX zeolites. Synthetic 0.05CaNaX-250 zeolite (calcined at 250 °C and Ca loading of 1.58 wt%) guarantees at least 21 Ca(OH) + species (depicted as hydroxylated Ca 2+ species) in the supercages per FAU cell unit, close to theoretical value. Such sorbent apparently improves the CO 2 uptakes and the separation from CO 2 /N 2 and CO 2 /CH 4 , along with fast kinetics, low heat of adsorption, measured by dynamic and gravimetric adsorption methods, respectively. In addition, it keeps a superior recyclability after 10 times regeneration. CO 2 -dosing FTIR experiments further illustrate that excellent CO 2 adsorption performance are benefited from the formation of Ca(OH) + ∙∙∙(CO 2 ) 2 adducts with an appropriate interaction. This work is of great significance to better understand the role of cations in FAU zeolites, and also provides an important reference value for the directional design of effective adsorption sites in other excellent CO 2 zeolite sorbents.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
危险品化学品经营许可证（带存储）