Surfaces and Interfaces
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2023
·
IF 6.2
Ning Liu,Bin Hu,Kexin Tang,Tingyu Xia,Fei Li,Guixiang Quan,Xiaodong Zhang,Liang Tang
In the pursuit of restoring and preserving our planet's natural equilibrium, the development of photocatalytic agents with exceptional aptitude for CO 2 reduction stands as an essential undertaking, which would be greatly facilitated with the energy regeneration and environmental purification. Herein, a composite material HTiNbO 5 /UiO-66 (UTi) was amalgamated by a one-step solvothermal method. The resultant composite material exhibited remarkable improvement on the photoreduction efficiency of CO 2 reduction compared with pristine UiO-66 and HTiNbO 5 . Impressively, UTi composite with 3 wt% HTiNbO 5 (UTi-3) illustrated the highest CO 2 photoreducation activity to CO, the CO yield of UTi-3 was about 9.3 and 11.2 times higher than that of pure UiO-66 and HTiNbO 5 , respectively. The significantly improved photocatalytic performance could be ascribed to the enlargement of specific surface area, the improved visible-light absorption range and shrinkage of the energy band gap, which can increase photogenerated electron production to promote the reduction reaction of CO 2 to CO. The insights obtained from this study can guide the application of semiconductor composites in the field of CO 2 photocatalytic reduction, so as to design high efficiency photocatalysts .
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FUEL
·
2023
·
IF 7.4
Shanlong An,Xin Huang,Nuo Li,Qiangwei Li,Rujie Wang,Tieyue Qi,Lidong Wang
The CO 2 capture process based on amine absorption–regeneration is currently the most widely used technology, and the performance of absorbent is the key to this process. Biphasic absorbents have attracted considerable interest because of their strong potential to reduce the regeneration energy consumption and equipment investment costs. The mixed solution of diethylenetriamine (DETA) and 2-diethylaminoethanol (DEEA) has been proven to be a biphasic absorbent, but there is still a lack of comprehensive performance evaluation data. In this study, the ratio of the DETA/DEEA solution was optimized as 2 M DETA + 3 M DEEA, and its phase separation property, reaction mechanism, mass transfer kinetics, and desorption thermodynamics were investigated under various conditions. The comprehensive performance of the solution was then evaluated by further analyzing its oxidative degradation, thermal degradation, and metal corrosion characteristics. On this basis, the capital cost and operation cost of using DETA/DEEA biphasic absorbent were analyzed. Under typical coal-fired flue gas (CO 2 concentration 12%), because of the high CO 2 absorption capacity and excellent phase separation property, the minimal desorption energy consumption of the DETA/DEEA absorbent decreased to 2.14 GJ/t CO 2 , a 43.7% decrease compared with that of 5 M monoethanolamine (MEA). Under the same experimental conditions, DETA/DEEA exhibited an oxidative degradation rate of only 2.71%, which was 20.7% of 5 M MEA. In addition, the metal corrosion rate of DETA/DEEA was one order of magnitude lower than that of 5 M MEA. However, under a high CO 2 loading, its thermal degradation resistance needed to be improved, and it was clear that the rates of oxidative degradation, metal corrosion, and thermal degradation of the CO 2 rich lower phase were higher than those of the CO 2 lean upper phase. The capital cost and operational capture cost of the DETA/DEEA biphasic process were approximately $107.8/t CO 2 and $31.6/t CO 2 , respectively, which were 2.5% and 36.4% lower than those of the MEA process. These findings provide a theoretical basis for the industrial application of DETA/DEEA.
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CHEMOSPHERE
·
2023
·
IF 8.8
Lingfei Liu,Mingshan Zhang,Yi Lu,Gaojian Chen,Binda Lu,Lingling Ge,Zhouguang Lu,Dejun Sun,Zhenghe Xu
CO 2 -responsive microemulsion (ME) is considered a promising candidate for deep-cleaning and oil recovery from oil-contaminated soils. Understanding the responsive nature of different microstructures ( i.e. , oil-in-water (O/W), bicontinuous (B.C.) and water-in-oil (W/O)) is essential for unlocking the potential and mechanisms of CO 2 -responsive emulsions in complex multiphase systems and providing comprehensive guidance for remediation of oil-contaminated soils. Herein, the responsiveness of microstructures of ME to CO 2 trigger was investigated using experimental designs and coarse-grained molecular dynamic simulations. MEs were formed for the first time by a weakly associated pseudo-Gemini surfactant of indigenous organic acids (naphthenic acids, NAs are a class of natural surface-active molecules in crude oil) and tetraethylenepentamine (TEPA) through fine tuning of co-solvent of dodecyl benzene sulfonic acid (DBSA) and butanol. The O/W ME exhibited an optimal CO 2 -responsive character due to easier proton migration in the continuous aqueous phase and more pronounced dependence of configuration on deprotonated NA ions. Conversely, the ME with W/O microstructure exhibited a weak to none responsive characteristic, most likely attributed to its high viscosity and strong oil-NA interactions. The O/W ME also showed superior cleaning efficiency and oil recovery from oil-contaminated soils. The results from this study provide insights for the design of CO 2 -responsive MEs with desired performance and guidance for choosing the favorable operating conditions in various industrial applications, such as oily solid waste treatment , enhanced oil recovery (EOR), and pipeline transportation. The insights from this work allow more efficient and tailored design of switchable MEs for manufacturing advanced responsive materials in various industrial sectors and formulation of household products.
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高影响因子
Gels
·
2023
·Vol. 9
·期 9
·703
·
IF 4.6
Kaibo Xu,Liqin Cao
Herein, a green, carbon dioxide-in-water high-internal-phase emulsion (C/W HIPEs) was developed and stabilized with polyvinyl alcohol (PVA) for the formation of chitosan oligosaccharide/poly(acrylamide-co-sodium 4-styrene sulfonate) [COS/P(AM-co-SSS)] monolithic porous hydrogel. The obtained monolith was characterized via FT-IR and SEM. The SEM patterns depicted that the monoliths were interconnected, the void sizes were 78.5 µm, and the interconnected pore throats were 28 μm approximately. Mechanical measurement results indicated that the maximum compress stress of the monolith could reach 334.4 kPa at 90% strain, and it exhibited good mechanical stability. After 200 cycles of compression, it could still recover its original shape without cracking. The obtained COS-based monolith was selected to remove tetracycline (TC) for evaluating the adsorptive features of the interpenetrating pore-containing monolith. The monolithic COS/P(AM-co-SSS) hydrogel behaved with strong antibiotic adsorption capacity (1600.4 mg/g for TC). The adsorption process agreed well with the pseudo-second-order kinetic and Langmuir isothermal models. In addition, the porous monolith had a strong electrostatic force on TC according to the thermodynamic study. This work provides a green route for the development of novel monolithic hydrogels and highlights its potential application in the treatment of antibiotic-containing wastewater.Keywords:high-internal-phase emulsion;CO2-in-water;chitosan oligosaccharides;monolith;porous;hydrogel
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Xiaofeng Lai,Song Wang,Ying Xie,Binghang Liu,Jianhui Sun,Yuxin Li,Haitao Yu,Kai Pan
CsPbBr3 perovskite nanocrystals have emerged as promising candidates for photocatalysis. However, their conversion efficiency is hampered by material instability, and the accumulation of deactivated perovskites produced after photocatalytic reactions raises significant environmental concerns. To address this issue, we developed a mechanochemical grinding approach assisted by oleylamine as an additive to restore the optical properties and photocatalytic activity of deactivated CsPbBr3, which was due to aggregation in the photocatalytic CO2 reduction reaction. Upon regeneration, the CsPbBr3 nanocrystals exhibited an average length of 34.21 nm and an average width of 20.86 nm, demonstrating optical properties comparable to those of the pristine CsPbBr3 nanocrystals. Moreover, they achieved a conversion efficiency of 88.7% compared with pristine CsPbBr3 nanocrystals in the photocatalytic CO2 reduction reaction. This method effectively enhanced the utilization of CsPbBr3, offering a novel approach for the recycling and recovery of perovskite materials and thereby minimizing material waste and environmental pollution.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Yuhuan Wang,Jianyu Qiao,Shuqing Dong,Shijun Shao,Dengchao Wang
The detection of heavy metal ions Co 2+ is of great significance to the environment and human health. Herein, a simple, highly selective and sensitive photoelectrochemical detection strategy for Co 2+ was developed based on the enhanced activity by nanoprecipitated CoPi on the Au nanoparticle decorated BiVO 4 electrode. The new photoelectrochemical sensor has a low detection limit of 0.03 μΜ and wide detection range of 0.1–10, and 10–6000 μΜ, with a high selectivity over other metal ions . The Co 2+ concentration in tap water and commercial drinking water has also been successfully determined with the proposed method. Scanning electrochemical microscopy technique was employed to characterize the photocatalytic performance and heterogenous electron transfer rate of electrodes in situ, further revealing the photoelectrochemical sensing mechanism. Besides determining Co 2+ concentration, this approach of enhanced catalytic activity by nanoprecipitation can be further extended to develop a variety of electrochemical, photoelectrochemical and optical sensing platforms for many other hazardous ions and biological molecules.
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Fuying Zhu,Haochen Qiu,Fei Wang,Xing Zhang,Guo-Ping Lu,Yamei Lin,He Huang
CO2 conversion by stable, cost-effective carbonic anhydrase (CA)-like nanozymes emerges as an efficient and sustainable approach for CO2 fixation. In this work, a novel iron-based nanomaterial (Fe10@CN-Mg) was first reported to be a CA mimic, in which FeNx sites and Mg(OH)2 play a synergistically catalytic effect for CO2 conversion. Although this material has much lower metal content and cost, it has comparable kinetic constants (Km 6.37 mM and Vmax 30.74 mM/min) and a significantly higher CaCO3 formation rate (20.60 g·g–1·h–1, the quality of CaCO3 produced per hour per gram of the catalyst) than that of reported CA mimics. Fe10@CN-Mg is stable when processed at extreme pH, high temperature, organic solvents, and high ionic strength and also retains high activity after long storage times (two months) and seven cycles. In addition, Fe10@CN-Mg was successfully applied to convert CO2 into cyclic carbonates with high economic efficiency.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Rui Zhang,Ruixi Liu,Francesco Barzagli,Meher Geetika Sanku,Chao'en Li,Min Xiao
Mixing different amines is a common method to develop better solvents for CO 2 capture. As the mixing provides more adjustability on the solvent properties, it introduces complex interaction between dissimilar amine molecules who may perform diverse role in the reactions. Here we studied CO 2 absorption in monoethanolamine (MEA), methyldiethanolamine (MDEA) and their mixtures thereof. The speciation profiles along with CO 2 loading were provided via NMR to reveal the competition/coordination of MEA and MDEA in participating the key reactions that drove CO 2 absorption (i.e. carbamate formation and amine protonation). Furthermore, the CO 2 loading of the solvents were measured under equilibrium for various temperature, CO 2 partial pressure. The excessive CO 2 loading was firstly introduced to analyze the loading data regarding the solvent composition. Accordingly, an excessive property model was applied for data correlation. The calculated CO 2 loading agreed well with experimental data with average absolution relative deviation of 1.7%.
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Catalysts
·
2023
·Vol. 13
·期 5
·807
·
IF 3.9
Zhiping Zhao,Zhixia Wang,Yanbing Tong,Jinru Sun,Ming Ke,Weiyu Song
The search for inexpensive, environmentally friendly, and highly effective catalysts to activate C-H bonds in propane dehydrogenation (PDH) reactions is still a major challenge. Co-based catalysts have gained significant attention in recent years due to their excellent ability to activate C-H bonds and their high selectivity towards olefins, despite being a non-noble and environmentally unfriendly metal. However, further improvements are necessary for practical utilization, particularly in terms of activity and anti-carbon deposition capacity. In this study, we synthesized Al2O3nanorods with abundant pentacoordinated Al3+(Al3+penta) sites. The supported Co on the Al2O3nanorod (Co/Al2O3-NR) exhibited higher selectivity (>96% propylene selectivity) and stability (deactivation rate 0.15 h−1) compared to Co supported on an Al2O3nanosheet with fewer pentacoordinated Al3+sites. Various characterizations confirmed that Co(II) mainly exists as CoAl2O4rather than Co3O4in the form of Co/Al2O3-NR, which inhibits the reduction of Co(II) to Co0and accordingly improves catalyst stability.Keywords:propane dehydrogenation;metal oxide;alumina;spinel
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高影响因子
Journal of Coatings Technology and Research
·
2023
·Vol. 20
·期 5
·1569-1578
·
IF 2.3
Ding Zhu,Chen Jiahui,He Zonglin,Wang Chaozhi,Li Hualin,Huang Zhenhong,Liu Baohua,Song Lina
A series of two-component UV-curable waterborne CO 2 -based polyurethane dispersions (UV-PUDs) with excellent flexibility and mechanical strength were synthesized from poly(propylene carbonate) diol (PPCD), isophorone diisocyanate (IPDI), 2,2-bis(hydroxymethyl) propionic acid (DMPA), 2-hydroxyethyl acrylate (HEA), pentaerythritol triacrylate (PETA) and 1,4-butanediol (BDO). One component was UV-curable waterborne polyurethane terminated by HEA and PETA (molar ratio 1:1), and the other component was linear waterborne polyurethane. The content of the UV-curable component in UV-PUD was 15%, 30%, 45%, 60%, and 100% (weight content). The obtained cured films exhibited superior flexibility without loss of tensile strength, accompanied by excellent acid and alkali resistance. In particular, the dried UV-PUD films without curing showed good mechanical properties.
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RSC Advances
·
2023
·Vol. 13
·期 21
·14554-14564
·
IF 3.9
Zhong Xie,Jinpei Hei,Chuan Li,Xiaojie Yin,Fengyi Wu,Lei Cheng,Sugang Meng
An activated carbon-supported Cu/ZnO catalyst (CCZ-AE-ox) was successfully obtained by the ammonia evaporation method for the hydrogenation of carbon dioxide to methanol, and the surface properties of the catalyst post-calcination and reduction were investigated. Activated carbon facilitated the increased dispersion of the loaded metals, which promote the CO2 space-time yield (STY) of methanol and turnover frequency (TOF) on the active sites. Furthermore, the factors affecting the catalyst in the hydrogenation of CO2 to methanol were in-depth investigated. The larger surface area and higher CO2 adsorption capacity are found to make possible the main attributions of the superior activity of the CCZ-AE-ox catalyst.
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Journal of Energy Chemistry
·
2023
·
IF 13.1
Jing Zhang,Jia-Jun Dai,De-Quan Cao,Heng Xu,Xing-Yu Ding,Chun-Hua Zhen,Beate Paulus,Jin-Yu Ye,Qian Liang,Jun-Ke Liu,Shi-Jun Xie,Sai-Sai Deng,Zhen Wang,Jun-Tao Li,Yao Zhou,Shi-Gang Sun
With tunable local electronic environment, high mass density of MN 4 sites, and ease of preparation, metal–organic conjugated coordinative polymer (CCP) with inherent electronic conductivity provides a promising alternative to the well-known M−N−C electrocatalysts. Herein, the coordination reaction between Cu 2+ and 1,2,4,5-tetraaminobenzene (TAB) was conducted on the surface of metallic Cu nanowires, forming a thin layer of CuN 4 -based CCP (Cu-TAB) on the Cu nanowire. More importantly, interfacial transfer of electrons from Cu core to the CuN 4 -based CCP nanoshell was observed within the resulting CuTAB@Cu, which was found to enrich the local electronic density of the CuN 4 sites. As such, the CuTAB@Cu demonstrates much improved affinity to the *COOH intermediate formed from the rate determining step; the energy barrier for C–C coupling, which is critical to convert CO 2 into C 2 products, is also decreased. Accordingly, it delivers a current density of −9.1 mA cm −2 at a potential as high as −0.558 V (vs. RHE) in H-type cell and a Faraday efficiency of 46.4% for ethanol. This work emphasizes the profound role of interfacial interaction in tuning the local electronic structure and activating the CuN 4 -based CCPs for efficient electroreduction of CO 2 .
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