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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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
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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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DOI
高影响因子
RSC Advances
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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
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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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
ENERGY & FUELS
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2024
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IF 5.2
Bo Zhang,Chunming Xu,Quan Shi,Yiqiang Li,Zheyu Liu,Jianxun Wu
Supercritical CO2 flooding is an efficient method of enhanced oil recovery in which CO2 injection can selectively extract light components and cause the deposition of residue heavy components in reservoir pores. Residues can change the wettability of the rock surface to ultimately reduce crude oil production. In this study, supercritical CO2 extraction experiments were conducted under identical operation conditions using various minerals, including quartz, montmorillonite, Illite, dolomite, albite, calcite, and chlorite. The crude oil, extracts, and residues were comprehensively characterized using high-temperature gas chromatography and high-resolution mass spectrometry. The results indicate that the extraction effect is influenced by the specific surface areas and adsorption strengths of various minerals. The larger the specific surface area, the more readily the heteroatoms in the resins can be adsorbed onto the rock surface. Quartz exhibits weak adsorption strength toward heteroatoms, whereas minerals with high specific surface areas demonstrate significantly higher adsorption strengths compared to those with lower specific surface areas. The wettability changes of various mineral surfaces were also assessed through contact angle measurements. Upon exposure to crude oil, a rock surface undergoes a transition from being water-wet to becoming oil-wet. Subsequently, it reverts back to being more water-wet due to supercritical CO2 extraction which further proves the feasibility of alleviating channeling by injecting water. Furthermore, the alteration in wettability caused by the change in the carbon number of different heteroatoms under supercritical CO2 extraction is also investigated. This study provides a basis for the mechanism study of CO2–crude oil–rock interaction and a comprehensive understanding of the wettability alteration of different reservoirs in carbon dioxide flooding.
研究领域:
石油工程
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化学工程
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2025
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IF 2.5
Xiaoqi Jin,Zong-Qun Li,Jinlong Ge,Linlin Zhu,Caiyan Liu,Qiu Li,Jing Liu,Chenlin Yin,Gaoyu Su
Ca-based MOFs and related derived materials offer promising potential for CO2 capture. In this study, we synthesized a CaBTC MOF and polydopamine coated MOF composite by using an ultrasonic irradiation method, and a corresponding derivate was obtained by thermal treatment. The capacity of CO2 capture and subsequent adsorption performance from the resulting CaBTC MOF/MOF derivate under different temperatures were investigated in detail. The structural features and textural parameters of the obtained absorbents were assessed by XRD, SEM, EDS, FT-IR spectroscopy, Raman spectroscopy, XPS, TG-DSC, and N2 absorption/desorption characterization. The results demonstrated that the prepared of CaO/CN-x with basic functional groups exhibited micro/mesoporosity derived from organic matter removal through carbonization at 800°C. Both of these properties accounted for the highest CO2 capacity of 2.30 mmol/g at 273 K using pure CO2 for the CaO/CN-5 sample. Additionally, we found that the derivate of CaBTC MOF at high temperatures experienced two stages of chemical adsorption, as well as carbonation reaction. The high CO2 capture capacity reached 60.2 mass% in 10 min at 873 K for the CaO sample. Furthermore, the introduction of carbon components derived from organic matter in the CaBTC MOF derivate matrix promoted the conversion of CO2 to CO through the reduction reaction. Possible reaction mechanisms for the conversion of CO2 to CO were preliminary proposed based on thermodynamic calculation.
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
Journal of Sustainable Metallurgy
·
2023
·Vol. 9
·期 2
·588-598
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IF 2.4
Chai Xin,Meng Fan-Cheng,Zhang Xiang-lan,Zhang Xu-kun,Sun Linquan,Wang Lina
Owing to the high Na/V molar ratio of Na 3 VO 4 solution, traditional precipitation of vanadium will consume more H 2 SO 4 and discharge ammonia–nitrogen wastewater with more Na 2 SO 4 . In present work, a new process was proposed, in which CO 2 was employed to carbonate Na 3 VO 4 solution with simultaneous recovery of NaHCO 3 , followed by NH 4 VO 3 precipitation and solution recycling. Carbonation kinetics of Na 3 VO 4 solution under both atmospheric and high pressures were studied. Under atmospheric pressure, the solution pH first decreased rapidly, slowly, rapidly again with carbonation time, and finally stabilized at pH 7.3; the formation of CO 3 2− and its conversion to HCO 3 − mainly occurred and the CO 2 absorption rates of different vanadium concentrations were almost the same (about 0.026 mol·m −3 ·s −1 ) at pH of 9.0‒9.6. Under high pressure, the reaction rates at early stage increased with CO 2 pressure and vanadium concentration, and stirring speed had the most significant effect on reaction rate with the highest CO 2 absorption rate of 1.73 mol·m −3 ·s −1 at 550 rpm. The average CO 2 utilization efficiency was ~ 90% with NaHCO 3 precipitation of 42.3% at 70 g·L −1 V under 1 MPa of CO 2 pressure, while the average CO 2 utilization efficiency was ~ 35% under atmospheric pressure. Finally, the reaction rate equation of carbonation under high-pressure was deduced. Graphical Abstract
研究领域:
化学工程
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环境科学
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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
VACUUM
·
2025
·
IF 3.9
Jingwen Meng,Xiaoli Jin,Mengyuan Zhao,Zhuohua Chen,Weixi Hao,Shilong Lin,Xin Li,Fengyun Su,Fei Li,Kaiting Yang,Xiongtao Lv,Xuhan Zhang,Haiquan Xie
Limited light absorption and low carrier separation efficiency remain major obstacles to converting CO 2 into solar fuel. Rational design of semiconductor photocatalysts with unique structures holds promise for overcoming these challenges. In this study, Bi 4 O 5 Br 2 photocatalyst with a hollow core-shell architecture is synthesized via a one-step solvothermal method. This innovative structure facilitates efficient reflection and absorption of incident light within its internal cavity, while also minimizing the charge transfer path. Consequently, it significantly improves both light harvesting capabilities and charge carrier separation efficiency. Compared to the solid Bi 4 O 5 Br 2 (CO, 0.21 μmol g −1 h −1 ; CH 4 , 0.78 μmol g −1 h −1 ) and hollow Bi 4 O 5 Br 2 (CO, 0.25 μmol g −1 h −1 ; CH 4 , 0.99 μmol g −1 h −1 ) counterparts, the hollow core-shell Bi 4 O 5 Br 2 exhibits superior CO 2 photoreduction performance, achieving production rates of 3.61 and 2.40 μmol g −1 h −1 for CO and CH 4 , respectively. Notably, it also enhances C 2 H 4 production during the CO 2 reduction process, with a yield of 0.17 μmol g −1 h −1 , whereas no detectable C 2 H 4 is produced by either the solid or hollow Bi 4 O 5 Br 2 structures. This research provides fresh insights into the structural design of advanced photocatalysts and holds significant implications for converting CO 2 into high-value chemicals.
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
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Jing Lei,Wei Bi,Mitang Wang,Hao Jiang,Yanjie Hu,Chunzhong Li
How to achieve controllable preparation of heterostructure and in-situ optimize the interface and internal electron transfer by a fast and economic synthesis method has become a big challenge in the practical application of photocatalysis. Herein, an island-shaped SrTiO 3 (STO) perovskite nanodots and TiO 2 (T) compounded S-scheme SrTiO 3 /TiO 2 (ST) heterostructure was successfully developed. During the millisecond reaction process, the decomposed Sr 2+ penetrated into the TiO 2 lattice causing the lattice expansion and inducing local atomic rearrangements, resulting in the generation of STO phase. Owing to the synergy of the efficient electron transport at the perovskite nanodots interface and the stronger reduction capacity, the performance of the optimized ST1 sample is greatly improved to 86.90 μmol g −1 for CO 2 -to-CO and 21.31 μmol g −1 for CO 2 -to-CH 4 . The utilization of electrons reached up to 119.74 μmol g −1 h −1 , which was 3.13 times higher than that of T. Detailed characterizations and density functional theory (DFT) calculations proof that the formation of intermediates HCOO − and CO 3 2− is the key to the performance improvement critically. Overall, this work originally reports a feasible strategy for flame synthesis of S-scheme heterostructure photocatalyst.
研究领域:
光催化
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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
危险品化学品经营许可证（带存储）