CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yetong Li,Kailong He,Siyuan Zhao,Linyu Jiao,Huiyong Chen,Xiaoxun Ma,Chengyi Dai
Many researchers have extensively studied the alkylation of naphthalene with methanol for the preparation of high-value-added chemicals, especially methylnaphthalenes (MNs). Studies indicated that methanol generates a large number of methanol-to-olefin by-products on zeolites, resulting in low selectivity of the target product and poor stability of the catalyst, limiting its application in the industrial field. In this study, CO 2 hydrogenation was coupled with naphthalene alkylation, and the H 3 CO* active intermediate generated in situ was alkylated with naphthalene by using metal oxide-zeolite (OX-ZEO) bifunctional catalysts, which exhibited the ‘slow release’ phenomenon of the methylation reagent. It improved naphthalene conversion, suppressed deep alkylation and coke deposition side reactions and kept the catalyst stable for up to 500 h. A high-density and medium-strength Brønsted acid center facilitated the efficient migration of H 3 CO* active intermediates with the desorption of 2-methylnaphthalene (2-MN), which was particularly important for improving naphthalene conversion and 2-MN selectivity. The in situ IR showed that more Brønsted acid sites of Ga-S-1 effectively pulled the migration process of H 3 CO* species to the zeolitic acid center and increased the efficiency of C-C coupling compared to ZSM-5, which promoted the alkylation of H 3 CO* species with naphthalene. The results of chemisorption experiments showed that the medium-strength Brønsted acid site, which promoted the desorption of 2-MN, inhibited the deep alkylation reaction. The 2,6-dTBPy-IR results showed that the presence of fewer Brønsted centers on the outer surface of Ga-S-1 further optimized the product distribution and enhanced the selectivity of 2-MN in MNs to more than 90 %. Under optimal conditions, 80.1 % selectivity for MNs was obtained via ZnZrO x &Ga-S-1 bifunctional catalysts, with 97.4 % selectivity for 2-MN in MNs.
✓ 已验证
产品关联
DOI
高影响因子
MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Yanfei Wang,Tongge Li,Shihui Wang,Xiao Du,Lin Li,Hui Xiao,Zhaoyuan Zhang,Feiyang Jiang,Shifa Li,Zhenzhong Wang,Yifang Wang,Ning Yang
The excessive emission of industrial CO 2 seriously threatens the living environment of human beings. In this paper, we propose a CO 2 sensing method based on cyclic microfluidic and dynamic flow detection technology. Firstly, a microflow permeation model was established to describe the numerical relationship between CO 2 permeation flux and gas phase inlet concentration and velocity. Secondly, we designed a microfluidic chip with coupled gas–liquid circulation and optimized its channel structure. Based on this, a microflow fluorescence response sensing system was built to analyze the fluorescence response spectral characteristics under different CO 2 permeation fluxes. Then, the optimal gas flow rate selection strategy for different CO 2 concentrations was proposed, and the CO 2 dynamic sensing model was established. Finally, the reliability of the proposed detection method is verified by comparing the detection results of commercial sensors with standard gases. The results indicate that the linear correlation coefficient between the relative fluorescence intensity and CO 2 concentration of the proposed CO 2 dynamic sensing method is 0.9987, the detection error of low concentration range is 193.3 ppb, and the detection error of high concentration range is less than 193.3 ppm. Compared with the parallel flow mixing device, the gas–liquid circulation-coupled microfluidic chip designed in this paper has better gas–liquid mixing effect. The system can operate continuously in the air for 40 weeks. Compared with commercial sensors, it has the advantages of better reusability, high linearity and low detection error in the whole range.
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-10
·
IF 15.7
Zhang Zhiyong,Wang Yang,Xie Yangen,Tsukamoto Toru,Zhao Qi,Huang Qing,Huang Xingmiao,Zhang Boyang,Song Wenjing,Chen Chuncheng,Sheng Hua,Zhao Jincai
To enable open environment application of artificial photosynthesis, the direct utilization of environmental CO 2 via an oxygen-tolerant reductive procedure is necessary. Herein, we introduce an in situ growth strategy for fabricating two-dimensional heterojunctions between indium porphyrin metal-organic framework (In-MOF) and single-layer graphene oxide (GO). Upon illumination, the In-MOF/GO heterostructure facilitates a tandem CO 2 capture and photocatalytic reduction on its hydroxylated In-node, prioritizing the reduction of dilute CO 2 even in the presence of air-level O 2 . The In-MOF/GO heterostructure photocatalyst is integrated with a porous polytetrafluoroethylene (PTFE) membrane to construct a floatable artificial leaf. Through a triphase photocatalytic reaction, the floatable artificial leaf can remove aqueous contaminants from real water while efficiently reducing CO 2 at low concentrations (10%, approximately the CO 2 concentration in combustion flue gases) upon air-level O 2 . This study provides a scalable approach for the construction of photocatalytic devices for CO 2 conversion in open environments.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Meisi Chen,Weida Chen,Bin Jiang,Ying Huang,Tong Lei,Feng Zhang,Youting Wu
An amino acid based ionic liquid ([N 1111 ][Ala]) was employed as a trigger to start the phase separation of 2-(2-aminoethylamino) ethanol (AEEA) and 1-ethylimidazole (Eim) solutions (AEH) and to enhance CO 2 capture. Due to the accompanying phase change, the CO 2 load of AEEA-Eim-H 2 O-[N 1111 ][Ala] (AEHI) is 1.47 times higher than that of AEH. The interaction mechanism between AEHI and CO 2 was elucidated by spectroscopic analysis and molecular simulation. The water-shell layer around [Ala]–CO 2 and hydrogen-bonding were first proposed and demonstrated to be the key reasons for the phase separation. The formation of the water-shell layer expelled Eim from the rich phase and thus facilitated the proton transfer process, which not only accelerated the phase separation process but also reduced the regeneration energy consumption. After successive absorption–desorption cycles, the CO 2 uptake decreased slightly. The innovative mechanism provides important guidance for the design of excellent biphasic absorbents with good performance and low energy consumption.
✓ 已验证
产品关联
DOI
高影响因子
MACROMOLECULES
·
2024
·
IF 5.1
Yu Zhang,Feng Zhang,Shuqi Liu,Lele Guo,Zhenggong Wang,Jian Jin
High-performance polymer-based H2/CO2 separation membranes are attractive for sustainable blue hydrogen production. However, achieving high-flux separation remains a challenge, as H2 and CO2 have similar diffusion rates within the polymer. In this work, hydrogen-bonded polyamide (PA) network membranes are synthesized through interfacial polymerization involving Tröger’s base diamine (TBDA) and 1,3,5-benzenetricarbonyl trichloride, aiming to enhance the efficiency of H2/CO2 separation. Incorporating the contorted TBDA unit into the PA structure enhances microporosity, which, in turn, boosts the H2 permeance of the PA membrane. Notably, the presence of numerous intermolecular hydrogen bonds between N atoms in the TBDA and H atoms in the amide groups helps to restrict the pore size further, thereby improving the H2/CO2 selectivity of the membrane. The resulting PA membrane demonstrates an outstanding H2/CO2 selectivity of 23.5, coupled with a high H2 permeance of 160 gas permeation unit (GPU), significantly exceeding the current upper bound. Additionally, our PA membranes maintain a stable H2/CO2 selectivity of approximately 21.5 and a H2 permeance of around 160 GPU over 100 h, indicating excellent long-term stability. These findings suggest that the development of such advanced polymer membranes could pave the way for more efficient and sustainable blue hydrogen production, overcoming existing limitations in gas separation technologies.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Chenchen Weng,Cheng Wang,Yang Song,Yu-Xiao Zhang,Kang Zou,Hongwu Chen,Xue Yang,Wei Lin
The electrocatalytic CO 2 reduction reaction (CO 2 RR) to carbon-based fuels represents a promising strategy for carbon neutrality. Bi-based materials have emerged as leading candidates for CO 2 RR towards formate. However, dynamic reconstruction under actual CO 2 RR conduction imposes a challenge for the well-designed pristine Bi-based catalyst to deliver electrocatalytic activity. Herein, we report a high-efficient Bi catalyst which is in-situ formed via electrochemical activation of NO 3 − modulated Bi 2 O 2 CO 3 during CO 2 RR. The in-situ and ex-situ characterizations demonstrate that a directional reconstruction has been achieved under NO 3 − adjustment, in which the reinforced configuration focuses on the ordered Bi planar surface. The peak Faradaic efficiency for formate (FE HCOO − ) of 97 % is achieved at −0.9 V vs . RHE and a potential region with FE HCOO − over 90 % ranges from −0.7 to −1.1 V. Additionally, the formate partial current density reaches up to 329 mA cm −2 in a gas diffusion electrode configuration. The outstanding durability is evidenced through its stable and efficient formate production over 45 h. Moreover, the in-situ attenuated total reflection infrared and Raman analysis reveals that the *OCHO is the key intermediate for CO 2 RR towards formate and the in-situ generated Bi renders the favorable interaction with *OCHO intermediate, thus promoting CO 2 RR performance.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Zewei Hao,Ziyi Tian,Xinru Tian,Li Ma,Yuanzhe Gao,Mingfei Shao,Ruikang Zhang
Photocatalytic CO 2 reduction has drawn widespread attention across all sectors of society. Layered double hydroxides (LDHs) have emerged as promising photocatalysts, renowned for their adjustable bandgaps and reaction sites. As a typical anionic layered material, LDHs exhibit intricate interactions between interlayer anions and brucite-like metal layers, greatly influencing their inherent physicochemical properties. In this work, we synthesized ZnAl-LDH samples intercalated with four distinct anions: carbonate (CO 3 2– ), chloridion (Cl – ), nitrate (NO 3 – ), and dodecyl sulfate (DS – ), denoted as LDH-CO 3 , LDH-Cl, LDH-NO 3 , and LDH-DS, respectively. These LDHs samples have comparable crystallinity and morphology but differ in their interlayer spacing. XRD results reveal interlayer spacings of 0.77 nm for LDH-CO 3 , 0.78 nm for LDH-Cl, 0.88 nm for LDH-NO 3 , and 1.24 nm for LDH-DS, between adjacent brucite-like ZnAl hydroxide layers. Remarkably, LDH-NO 3 demonstrates the highest photocatalytic CO 2 reduction performance, with CO as the primary reduction product. Specifically, the average CO production rate of LDH-NO 3 are 3.80 μmol g –1 h –1 , surpassing that of LDH-CO 3 , LDH-Cl, and LDH-DS by 1.9, 2.1, and 2.5 times, respectively. This superior performance can be attributed to the intermediate interlayer spacing of LDH-NO 3 , which facilitates strong light absorption and a robust local built-in electric field. Theses properties enhance charge generation and separation abilities, leading to efficient photocatalytic reactions. The obtained results highlight the critical role of controlling small molecules within the interlayer, alongside defects, in the design and fabrication of layered-structure photocatalysts. This study provides valuable insights into optimizing the performance of LDH-based photocatalysts for CO 2 reduction and potentially other photocatalytic applications.
✓ 已验证
产品关联
DOI
高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2025
·
IF 7.8
Shaoxiong Song,Shiyu Dong,Yang Liu,Quanhua Xie,Yuanyuan He,Hassan Karimi-Maleh,Nianbing Zhong
In this study, a tube photocatalytic CO 2 reduction reactor was constructed to in situ online decode the surface CO 2 reduction rates of fixed photocatalysts. The photoreactor consisted of a hollow quartz tube with an inner surface coated with a composite photocatalyst of graphitic carbon nitride (g-C 3 N 4 ) and germanium dioxide (GeO 2 ). Subsequently, a fiber Bragg grating (FBG) CO 2 concentration sensor and its detection system were developed for online and accurate in situ detection of the CO 2 concentration on the surface of the photocatalytic film. The sensor system was then used to monitor the effect of the composition and loading of the photocatalyst on the CO 2 reduction rate inside the reactor, as well as operational parameters such as the light intensity and humidity. The results highlighted that the FBG CO 2 concentration sensor could accurately detect CO 2 concentration changes under variable temperature and humidity conditions, with a detection limit of 82 µM and a response time resolution of 102 s. Under the conditions of excitation light with a wavelength of 380–780 nm, light intensity of 50 W, GeO 2 /g-C 3 N 4 photocatalyst loading mass of 0.1 g, and a relative humidity of 90 % RH, the photocatalytic film exhibited high catalytic activity, achieving a CO 2 conversion produces CH 4 , CO and H 2 at rate of 0.37 mM/h. The research findings provide valuable insights for the design and optimization of CO 2 photocatalytic reduction devices, while also advancing the development of comprehensive on-site monitoring techniques for the photocatalytic CO 2 reduction process.
✓ 已验证
产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2025
·
IF 7.7
Ying Qian,Jie Zou,Xiaoqing Jiang,Jie Wang,Juan Zhou,Chu Cheng,Xin Zhang,Wenming He,Qinghui Jin,Jiawen Jian
Yttria-stabilized zirconia (YSZ)-based amperometric humidity sensors are highly promising for in situ detection of high-temperature flue ducts due to their excellent stability and durability under extreme conditions. However, selectivity remains challenging due to the co-electrolysis of H 2 O and CO 2 , as these compounds have similar electrolysis voltages. In this study, LaFeO 3 is proposed as a sensing electrode to reduce CO 2 electrolysis and improve selectivity in amperometric humidity sensors. Analysis indicates that the improved selectivity is likely due to LaFeO 3 ’s lower electrochemical activity. Furthermore, the proposed sensor exhibits good repeatability and acceptable long-term stability for high-temperature humidity detection.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Lixin Song,Guobin Liu,Zhenping Qu
CO 2 hydrogenation to methanol and/or dimethyl ether (DME) holds promise for mitigating greenhouse gas effects and addressing energy scarcity. However, the relationship between product selectivity and the collective nature of the catalysts remains ambiguous due to the intricate reaction network. Here, a series of Cu/Zn x Al y O z catalysts with different surface properties have been engineered by manipulating the Zn/Al ratio to achieve product controllability for CO 2 hydrogenation. The results unveil the pivotal role of the H 2 dissociation capability in governing CO 2 conversion, which is regulated by the concentration of Cu 0 species. Furthermore, the number of surface hydroxyl groups, the proportion of moderately strong basic sites and moderately strong acidic sites show desirable linear correlations with the selectivity of CO, CH 3 OH, and DME, respectively. Importantly, the ZnAl 2 O 4 -Al 2 O 3 or Cu-ZnAl 2 O 4 -Al 2 O 3 interface notably enhances moderately strong acidic sites, aiding methanol dehydration to DME. This work offers a comprehensive guide to the rational design of catalysts for oriented product synthesis from CO 2 hydrogenation.
✓ 已验证
产品关联
DOI
高影响因子
NANOTECHNOLOGY
·
2024
·Vol. 35
·期 19
·195605
·
IF 2.9
Shuo Wang,Haotian Yin,Lei Wang,Jing Ding,Jinfeng Zhang,Hui Wan,Guofeng Guan
Photocatalytic reduction of carbon dioxide is a technology that effectively utilizes CO2 and solar energy. Sodium niobate (NaNbO3) has received much attention in the field of photocatalysis due to its excellent photocatalytic properties. However, the application of NaNbO3 in the field of photocatalysis is still limited by poor reaction to visible light and easy recombination of photo-generated carriers. Heterojunction with g-C3N4 to construct core–shell structure can effectively improve the above problems. Combining the two can design a core–shell composite material that is beneficial for photocatalytic reduction of CO2. Herein, we prepared a core–shell heterojunction g-C3N4/NaNbO3 by uniformly impregnating urea on the surface of NaNbO3 chromium nanofibers with NaNbO3 nanofibers prepared by electrospinning as a catalyst carrier, and urea as a precursor of g-C3N4. The core–shell structure of g-C3N4/NaNbO3 was verified by a series of characterization methods such as XPS, XRD, and TEM. It was found that under the same conditions, the methanol yield of core–shell g-C3N4/NaNbO3 was 12.86 μmol·g−1·h−1, which is twice that of pure NaNbO3 (6.67 μmol·g−1·h−1). This article highlights an impregnation method to build core–shell structures for improved photocatalytic reduction of CO2.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ChemSusChem
·
2024
·
IF 7.5
Rui Yang,Xiaozhong Zheng,Hao Fu,Xinyue Cao,Yangguang Hu,Yiyin Huang
Graphical Cu 7 S 4 /Cu nanoflowers with strong CO 2 adsorption and abundant boundaries were developed by a facile thermal reduction, which underwent in situ dynamic restructuring during ECR to generate highly active S-doped Cu 2 O/Cu hybrid catalyst. Thermodynamic and experimental analysis revealed that the optimized adsorption of the HCOO * intermediate on S−Cu 2 O/Cu was regulated and surface H was suppressed by S-doping. The high activity for CO 2 -to-HCOOH attributed to the strengthen CO 2 adsorption, abundant boundaries at Cu 2 O/Cu interfaces, and the regulation of adsorption energy by S-doping Optimized catalytic properties and reactant adsorption energy played a crucial role in promoting CO 2 electrocatalysis. Herein, Cu 7 S 4 /Cu underwent in situ dynamic restructuring to generate S−Cu 2 O/Cu hybrid catalyst for effective electrochemical CO 2 reduction to formate that outperformed Cu 2 O/Cu and Cu 7 S 4 . Thermodynamic and in situ Raman spectra revealed that the optimized adsorption of the HCOO* intermediate on S−Cu 2 O/Cu was regulated and the H 2 pathway (surface H) was suppressed by S-doping. Meanwhile, Cu 7 S 4 /Cu nanoflowers created abundant boundaries for ECR and strengthened the CO 2 adsorption by inducing Cu. These findings provide a new perspective on synthetic methods for various electrocatalytic reduction processes.
✓ 已验证
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）