Journal of Coatings Technology and Research
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2023
·Vol. 20
·期 5
·1569-1578
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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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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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ENERGY & FUELS
·
2023
·
IF 5.3
Chen Huang,Ying Zhang,Shuofan Li,Quan Shi,Suoqi Zhao,Linzhou Zhang
With the escalating global energy crisis and burgeoning environmental concerns as a result of the accumulation of used lubricating oil, the urgency and economic potential of recycling this waste is undeniably critical. Conventional methods, such as distillation and hydrogenation, often stumble upon operational difficulties as a result of thermochemical decomposition, while advanced procedures, like molecular distillation and membrane separation, face industrial scale-up, owing to prohibitive costs and limited separation capabilities. Herein, this study heralds the emergence of supercritical CO2 (SC-CO2) extraction, which can exemplify superior efficacy in addressing these concerns. Leveraging the high solvency under extreme pressure and low-temperature conditions, SC-CO2 can selectively separate undesirable components, reducing coke formation and simplifying subsequent refining stages. The comprehensive analysis, conducted using gas chromatography–mass spectrometry and high-resolution mass spectrometry, revealed the selectivity of SC-CO2 toward saturates with a smaller molecular weight. On the basis of this analysis, the optimal extraction condition was determined. Implementing a two-stage process at 70 °C and 10–20 MPa, we effectively eradicated residual small molecules and large polar compounds, yielding an intermediate fraction rich in isoparaffins and 1–4 ring naphthenes with a carbon distribution of C25–40. Notably, the recovery rate of saturates was 60%. Critically, the removal rate of undesirable components in recycled lubricating oil is remarkably high, reinforcing the practical viability and exceptional advantages of SC-CO2 extraction for lubricating oil recycling as a sustainable and economically rewarding solution to pressing global energy and environmental predicaments.
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ACS Catalysis
·
2026
·
IF 13.6
Liu Meng-Nan,He Zhen-Hong,Chen Zhuo,Wang Sen-Wang,Ruan Miao,Luo Yanping,Wang Kuan,Wang Weitao,Wang Huan,Liu Zhao-Tie
Direct hydrogenation of CO 2 to liquid hydrocarbons (C 5+ ) at low temperature is a highly desirable but challenging transformation, as conventional catalysts typically operate at high temperatures via indirect pathways by producing and using a CO intermediate. In this work, we report an inverse ZrO 2 /Co catalyst that enables direct CO 2 hydrogenation to C 5+ hydrocarbons at a low temperature of 200 ° C. Under optimal conditions, the catalyst achieves a high CO 2 hydrogenation activity of 26.0 mmol CO2 ·g Co –1 ·h –1 with 58.9 C-mol % selectivity toward C 5+ liquid hydrocarbons and negligible CO formation. The inverse architecture of ZrO 2 /Co, wherein ZrO 2 nanoislands are dispersed over metallic Co 0 particles, concurrently not only enhances CO 2 adsorption and suppresses H 2 adsorption but also delivers a surface C/H ratio approximately 31 times higher than that of pristine Co 0 , thereby promoting chain growth. In situ DRIFTS reveals that the inverse catalyst generates abundant oxygen-containing intermediates (HCOO–, HCO 3 –, CH 3 O–, and CH 3 COO–), which are subsequently hydrogenated to CH x for chain growth over Co 0 sites. This work not only provides a low-temperature catalyst for direct CO 2 -to-C 5+ conversion but also establishes inverse oxide/metal interfaces as a general platform for tuning C–C bond coupling in CO 2 hydrogenation.
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JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Zemin An,Nan Ma,Yuanjie Xu,Hua Yang,Huibo Zhao,Lizhi Wu,Li Tan,Chao Zou,Fanchun Meng,Bin Zhang,Xiuyun Wang,Yu Tang
Harnessing the selectivity in catalytic hydrogenation of CO 2 is important for producing valuable chemicals. Herein, the shape dependency of the CO 2 hydrogenation on singly dispersed Ru/CeO 2 catalysts is investigated. CeO 2 of three shapes, including nanocube, nanooctahedron and nanorod, are prepared as the catalyst supports and assigned to the surface of (100), (111) and (110) crystal plane, respectively. The Ru/CeO 2 (nanorod) exhibits the highest selectivity to CO (97.6 %) at 350 °C, while the Ru/CeO 2 (nanocube) exhibits a mediocre selectivity to CO (41.4 %) but the highest CO 2 conversion. The shape of the CeO 2 support determines the electronic state of supported Ru atoms through the electronic metal-support interaction. The low CO affinity on cationic Ru β sites leads to the higher selectivity to CO on the Ru/CeO 2 (nanorod) and Ru/CeO 2 (nanooctahedron) catalysts, while the strong dissociation ability of H 2 on low valence Ru α sites results in the high activity on the Ru/CeO 2 (nanocube) catalyst.
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CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Tiantian Chen,Min Zhou,Zhiquan Zhang,Kai Yang,Xiaohong Fu,Huaming Li,Weidong Shi,Zhifeng Jiang
CO 2 Photoreduction through C–O bond cleavage and C–H bond formation has aroused as an alternative to fabricate high-value chemical fuels that are independent of fossil reserves. However, sluggish charge transfer and neglected light-induced heat utilization are thermodynamically and kinetically challenging. Herein, we subtly design a three-dimensional ultrathin composite consisting of flower-like ZnIn 2 S 4 (ZIS) and low-cost biochar (BC). The as-prepared ZIS/BC photocatalyst displays an optimized performance and stability toward CO 2 conversion, with a high CO yield of 20.7 μmol g −1 h −1 and a small yield of CH 4 , C 2 H 4 , and C 2 H 6 in comparison with ZIS and BC counterparts. This exciting activity originates from high electron conduction efficiency, light-harvesting ability, and the photothermal effect, which is produced from the intense interfacial contact of BC and ZIS. This work suggests that traditional photocatalysts can be elevated by inhibiting photocorrosion by introducing highly economical and electron conductivity biomass carbon in solar-induced green-chemical feedstock production.
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Molecular Catalysis
·
2023
·
IF 4.6
Zhishuai Wang,Fengyun Su,Hailong Cao,Mengzhen Tian,Xiang Li,Haiquan Xie,Xiaoli Jin,Zhengdao Li,Xin Ying Kong
Amidst the impending energy crisis and escalating concerns about global warming, photocatalytic reduction of carbon dioxide (CO 2 ) emerges as a promising solution. However, the practical application of this technology has been hindered by challenges such as the poor photoresponse of existing photocatalysts toward visible light, inefficient separation efficiency of photoinduced electron-hole pairs, and subpar product selectivity. This work simultaneously addresses these limitations by enhancing the activity of photocatalytic CO 2 reduction through the strategic incorporation of nickel oxide (NiO) onto niobium pentoxide (Nb 2 O 5 ). In this study, Nb 2 O 5 was prepared using the hydrothermal and calcination methods, culminating in the synthesis of NiO-supported Nb 2 O 5 achieved through the photodeposition method. The resulting 2 %-NIONBO photocatalyst with the optimal loading of NiO exhibited a remarkable methane (CH 4 ) production yield of 29.65 μmol/g/h, a striking 6.2-fold improvement over solitary NBO. In addition, the useful carbon monoxide (CO) fuel was also detected from the photoreduction of CO 2 , where 2 %-NIONBO exhibited a CO yield of 7.22 μmol/g/h, demonstrating a 3.4-fold enhancement over NBO, along with an outstanding CH 4 selectivity of 80.42 %. This study provides insights into the design and development of Nb-based photocatalysts for significantly enhanced efficiency in photocatalytic CO 2 reduction, paving the way for advancements in sustainable energy solutions and addressing environmental issues.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Lei Yuan,Leihao Zhang,Guilin Li,Shaojuan Zeng,Qizhou Xue,Chongyang Jiang,Xiangping Zhang
Electric-driven reduction of CO2 to high value-added chemicals is considered to be one of the most promising methods for CO2 utilization. In this work, a novel aprotic electrolyte consisting of phenoxy-nitrile bifunctional ionic liquid ([TBP][p-CN-PhO]) and acetonitrile was designed for CO2 electroreduction to oxalate, which shows the maximum Faradaic efficiency (FE) of 84.9% at −2.6 V. Importantly, a high oxalate formation rate of 233.7 μmol·cm–2·h–1 and oxalate FE of 73.9% were simultaneously achieved to break the trade-off effect at −2.8 V in the bifunctional ionic liquid electrolyte, which is also one of the state-of-the-art performances for CO2 electroreduction to oxalate. The significant performance of CO2 electroreduction was attributed to the strong interaction energies of phenoxy and nitrile groups with CO2 molecules in the bifunctional ionic liquid, which greatly facilitates CO2 activation to form CO2– radicals by a new bulk-phase pathway and then dimerizes into C2O42– at a lower energy barrier.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Zhiwei Jian,Jiangwei Yu,Ian Jimmy Madatta,Yang Liu,Jinrui Ding
The electrochemical reduction of carbon dioxide (CO 2 ) to high-energy multi-carbon compounds is a significant challenge. Efforts have been made to design efficient catalysts for high selectivity toward multi-carbon products. In this study, granular protruded irregular Cuprous oxide (Cu 2 O) nanoparticles were synthesized using a simple water bath wet chemical reduction method. Polyethylene glycol (PEG) was utilized as a directing agent to control the morphology of Cu 2 O in the process. The optimized irregular Cu 2 O (ir-Cu 2 O) catalyst exhibits a remarkable faraday efficiency of 69.3% (±3.3%) for double-carbon compounds (C 2 ), which is significantly higher than that of polyhedral Cu 2 O (p-Cu 2 O) (50.4%±1.1%) synthesized without adding PEG . Cu 2 O nanoparticles with irregular shape featuring randomly distributed spherical protrusions offer more active sites for CO 2 adsorption than p-Cu 2 O catalysts, which is beneficial for the conversion of CO 2 to C 2 . In addition, in situ infrared spectra reveal that ir-Cu 2 O reduces CO 2 to C 2 mainly through the coupling of the CO* and CHO*, thereby promoting the formation of C 2 . These findings provide valuable insights for the design of high-efficiency electrocatalysts for CO 2 electroreduction to C 2 .
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Chen Wang,Yan Zhu,Yihan Ling,Yansheng Gong,Rui Wang,Huanwen Wang,Jun Jin,Ling Zhao,Beibei He
Solid oxide electrolysis cells (SOECs) show great promise in converting CO2 to valuable products. However, their practicality for the CO2 reduction reaction (CO2RR) is restricted by sluggish kinetics and limited durability. Herein, we propose a novel medium-entropy perovskite, Sr2(Fe1.0Ti0.25Cr0.25Mn0.25Mo0.25)O6−δ (SFTCMM), as a potential electrode material for symmetrical SOEC toward CO2RR. Experimental and theoretical results unveil that the configuration entropy of SFTCMM perovskites contributes to the strengthened metal 3d–O 2p hybridization and the reduced O 2p bond center. This variation of electronic structure benefits oxygen vacancy creation and diffusion as well as CO2 adsorption and activation and ultimately accelerates CO2RR and oxygen electrocatalysis kinetics. Notably, the SFTCMM-based symmetrical SOEC delivers an excellent current density of 1.50 A cm–2 at 800 °C and 1.5 V, surpassing the prototype Sr2Fe1.5Mo0.5O6−δ (SFM, 1.04 A cm–2) and most of the state-of-the-art electrodes for symmetrical SOECs. Moreover, the SFTCMM-based symmetrical SOEC demonstrates stable CO2RR operation for 160 h.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Shuhui Xia,Chaolong Wei,Yong Zhai,Bin Ding,Jianyong Yu,Jianhua Yan
Photocatalytic CO 2 reduction is an attractive strategy to realize carbon–neutral economy but is challenging by its low efficiency and uncontrollable selectivity. Here, we report a new flexible black BaTiO 3 nanofiber (B-BTO NF) and prove its unique function of ultrasonic cavitation enhanced photocatalytic CO 2 reduction into controllable syngas. The B-BTO NFs with a large deformation ability and a high mechanical strength contain unsaturated Ti 3+ coordination and vacancy defects. Under ultrasound, the NF film gathers abundant cavitation bubbles, and the continual explosions of these bubbles bring periodic piezoelectric polarization changes and release net charges on B-BTO NFs, thus triggering photocatalytic CO 2 reduction into syngas. Moreover, the product selectivity can be controlled by facilely adjusting the ultrasonic frequency and power. As a result, the evolution rate of target syngas (CO/H 2 ≈ 1:1.3) reaches as high as 12525 μmol/g/h. The proposed flexible B-BTO NF induced ultrasonic cavitation-enhancement strategy provides new insights for designing photocatalysts.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-12
·
IF 16.6
Jiao Jiqing,Yuan Qing,Tan Meijie,Han Xiaoqian,Gao Mingbin,Zhang Chao,Yang Xuan,Shi Zhaolin,Ma Yanbin,Xiao Hai,Zhang Jiangwei,Lu Tongbu
Elucidating the synergistic catalytic mechanism between multiple active centers is of great significance for heterogeneous catalysis; however, finding the corresponding experimental evidence remains challenging owing to the complexity of catalyst structures and interface environment. Here we construct an asymmetric TeN 2 –CuN 3 double-atomic site catalyst, which is analyzed via full-range synchrotron pair distribution function. In electrochemical CO 2 reduction, the catalyst features a synergistic mechanism with the double-atomic site activating two key molecules: operando spectroscopy confirms that the Te center activates CO 2 , and the Cu center helps to dissociate H 2 O. The experimental and theoretical results reveal that the TeN 2 –CuN 3 could cooperatively lower the energy barriers for the rate-determining step, promoting proton transfer kinetics. Therefore, the TeN 2 –CuN 3 displays a broad potential range with high CO selectivity, improved kinetics and good stability. This work presents synthesis and characterization strategies for double-atomic site catalysts, and experimentally unveils the underpinning mechanism of synergistic catalysis.
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