Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Panpan Wang,Meiyu Shi,Yuan Shu,Qiang Niu,Pengfei Zhang
Daily discarded egg residues such as eggshells reach an astronomical figure around the world, causing severe environmental pollution and waste of Ca-based sources. CaCO 3 , especially these porous CaCO 3 nanoparticles, could role as an effective plastic stuffing, filler, ink filler, and adsorbent, having a great prospect for industrial application. Herein, based on a solid-state reaction between strong and weak acids, we successfully prepared a porous CaCO 3 -es with the BET specific surface area (SSA) up to 97.4 m 2 /g, and meanwhile with abundant mesopores and tiny small CaCO 3 primary nanoparticles about 7.4 nm. Notably, the prepared CaCO 3 -es showed significantly improved CO 2 adsorption capacity than the contrast CaCO 3 samples in both static and breakthrough tests. According to the characterization such as FTIR, Raman, XPS, TEM, and DFT calculations, the high CO 2 adsorption of CaCO 3 -es originated from its high porous structure, small nanoparticle size, and rich defective sites.
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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.
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JACS Au
·
2025
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IF 8.7
Xuan Bie,Yukun Pan,Xiaowei Wang,Shiyu Zhang,Jiahui Hu,Xiaoxiao Yang,Qinghai Li,Yanguo Zhang,Robert E. Przekop,Yayun Zhang,Hui Zhou
Gas sources rich in CO2 derived from biomass/waste gasification, anaerobic digestion, or industrial carbon capture often contain impurities such as H2S, H2O, and NH3, which can significantly hinder catalyst performance. Here, we show the role of NH3 on the reverse water–gas shift (RWGS) reaction over a commercial Cu/ZnO/Al2O3 catalyst, examining its effects on both the catalytic activity and the catalyst structure. We found that NH3 reversibly decreases CO2 conversion immediately by suppressing carbonate hydrogenation and CO desorption. This effect intensifies with an increase in NH3 concentration but decreases at higher temperatures. However, prolonged exposure (over 100 h) to RWGS conditions in the presence of 1.4% NH3 leads to near-total and irreversible deactivation of the Cu/ZnO/Al2O3 catalyst. Under NH3 exposure, the catalyst loses Cu+ sites on the surface, causing a spatial separation of Cu and ZnO. Finally, to address this challenge, we propose a novel strategy to mitigate NH3 inhibition by decomposing NH3 into N2 and H2.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jiale Wang,Shiyan Ma,Yun Huang,Ao Xia,Xianqing Zhu,Xun Zhu,Qiang Liao
Microalgae, as efficient photosynthetic autotrophs, hold significant potential for carbon sequestration. However, their photosynthesis is constrained by the selective use of the solar spectrum. To enhance the utilization of natural light energy, a dual functional substrate with ultraviolet (UV) light conversion and microalgae biofilm support was proposed by coating a rare earth complexes phosphor agent onto transparent acrylic in this study. By doing this, UV light could directly drive microalgae biofilm photosynthesis by converting it to red light, resulting in a maximum 2.81 times increase in the carbon fixation rate. The UV conversion substrate increased the electron transport rate of microalgal photosystem II by 58.08%, effectively enhancing the photosynthetic rate and oxygen release, promoting the formation of a porous biofilm structure, and strengthening the material transfer within the biofilm. Additionally, reactive oxygen species (ROS) can cause oxidative stress, affecting cell growth and metabolic activity. With the use of the UV conversion substrate, the levels of ROS and malondialdehyde (MDA) in microalgae decreased by 84.56% and 42.35%, respectively. Consequently, UV-induced damage to microalgae cells was reduced, leading to a 52.52% increase in the photosynthesis rate and achieving UV driven photosynthetic carbon sequestration. This study demonstrated the UV conversion substrate’s effectiveness in reducing UV-induced damage in microalgae and enhancing photosystem activity, showing significant potential for carbon fixation within microalgal biofilms.
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CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Ting Qu,Jinpeng Zhang,Jinbo Song,Jieying Jing,Wen-Ying Li
The magnesium oxide (MgO) sorbents doped with different NaNO 3 /NaNO 2 molar ratios were prepared to improve their stability over multiple cycles. Regulating the NaNO 3 /NaNO 2 molar ratio effectively improved the CO 2 adsorption performance of the sorbent. The MgO sorbent with the NaNO 3 /NaNO 2 molar ratio of 0.8 exhibited outstanding performance and stability. Characterization and density functional theory calculations confirmed the positive effects of the appropriate NaNO 3 amount in improving the adsorption activity, whereas the suitable NaNO 2 amount slowed the sintering step and improved stability. Notably, the molten salt remained stable during cycling and did not decompose even at high regeneration temperatures, guaranteeing the cyclic stability of the sorbent. Further characterization showed that the CO 2 sorption drop in the first few cycles was ascribed to the decline in the active surface owing to the aggregation of MgO particles, incomplete regeneration of sorbents, and segregation of molten salt on the sorbent surface.
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Nano Energy
·
2025
·
IF 17.1
Peng Bai,Jiafa Chen,Yicheng Zhao,Yongdan Li
CO 2 formylation of amines provides a promising route to convert CO 2 into value-added chemicals. That process is usually performed through a thermo-catalytic approach with additional reducing agents, which increases the energy consumption and the complexity of the system. Herein, we report photocatalytic CO 2 formylation of benzylamine over Pt 1 In-ZnO x single-atom-alloy catalyst at room temperature in N , N -dimethylformamide (DMF) solvent. The anchoring of Pt single atoms onto In nanoparticles through Pt-In bonds accompanied with electron transfer from In to Pt improves the absorption capacity for visible light and the separation efficiency of photogenerated charge carriers. Furthermore, the adsorption and activation of CO 2 and benzylamine are promoted on the surface of Pt 1 In single-atom-alloy. After 6 h reaction under visible-light, the yield of N -benzylformamide reaches 48.6 mmol g −1 with a 95.3 % selectivity. A possible reaction mechanism is proposed based on a series of in situ characterizations and theoretical calculations. A decomposition-regeneration cycle of DMF is involved in the photocatalytic process, which extends the reaction region and thus facilitates the formylation of benzylamine. The photocatalytic system exhibits good cycling stability and universality. This work provides new insights for the rational design of single-atom-alloy catalyst and an efficient approach for the sustainable utilization of CO 2 .
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Materials Today Communications
·
2024
·
IF 3.7
Zhihua Feng,Bo Tang,Kexin Liu,Qingqing Hou,Zhangting Dang,Cui Yang,Xiufu Hua,Qiushuo Yu,Lingling Wang,Renbo Wei
The chemical transformation of CO 2 into high-value-added products is not only favourable to environmental preservation, but also promising for economy. Developing novel and practical catalysts play a critical role in facilitating conversion of CO 2 and the synthesis of high value-added chemicals. Herein, we present the fabrication of biphenyl-typed copper phthalocyanine polymer (BPh-CuPc) from 4,4’-bis(3,4-dicyanophenoxy)biphenyl via a one-pot synthesis procedure, and application of it as a promising catalyst for CO 2 conversion into cyclocarbonate. FTIR, XPS, UV–vis, TGA and SEM measurements confirm the successful fabrication of BPh-CuPc. Attributing to the existence of copper ions which can act as a Lewis acid to activate epoxide, and phthalocyanine rings that is positive for CO 2 absorption, within the chemical framework of BPh-CuPc, it exhibits excellent catalytic activity for CO 2 conversion into cyclic carbonates under mild conditions when combined with tetrabutylammonium iodide (TBAI). As a result, a 98 % yield and 99 % selectivity are obtained for the BPh-CuPc/TBAI system in CO 2 /propylene oxide conversion under condition of 90 °C, 8 h and 2.0 MPa. The obtained high yield and selectivity, as well as remarkable stability and versatility, validate the promising application of BPh-CuPc as a CO 2 conversion catalyst. Synopsis Attributing to the existence of copper ions and phthalocyanine rings within the chemical framework, BPh-CuPc exhibits excellent catalytic activity for CO 2 conversion into cyclic carbonates under mild conditions.
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JOURNAL OF POLYMER RESEARCH
·
2025
·Vol. 32
·期 3
·1-9
·
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.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Xi Liu,Delong Hou,Demeng Liu,Siyu Pan,Jun Yan,Qi Zeng,Yi Chen
The α-methyl esterification of natural fatty acid methyl esters (FAMEs) is an essential approach for preparing high-value chemicals such as migration-resistant bioplasticizers, polyester precursors, and anionic surfactants. However, previous strategies are primarily based on time-consuming Claisen condensation, which utilizes petroleum-derived dimethyl carbonate (DMC) as a building block for α-methyl esterification, as well as a NaH/DMF deprotonation system with a highly explosive risk. Here, we present an efficient approach that harnesses carbon dioxide as a green C1 building block to facilitate rapid, nonexplosive α-methyl esterification of FAMEs, producing fatty acid dimethyl esters with high yield (>85%) at ambient temperature within 3 h. Various natural FAMEs, even those derived from waste cooking oil, are amenable to this approach. Our findings establish a robust strategy for α-methyl esterification of FAMEs, bringing the production of high-value chemicals from FAMEs one step closer to sustainability.
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ADVANCED MATERIALS
·
2025
·Vol. 37
·期 39
·2510192
·
IF 26.8
Haozhou Yang,Na Guo,Shibo Xi,Haiyuan Zou,Jiayi Chen,Lei Fan,Yukun Xiao,Qian He,Lele Duan,Pengfei Wei,Guoxiong Wang,Chun Zhang,Lei Wang
Carbon nanotubes (CNTs) are widely used as supports for immobilizing molecular electrocatalysts, such as for CO 2 reduction (CO 2 R), with π-π interactions often assumed to govern the catalyst immobilization. However, the nature of catalyst/CNTs interactions remains insufficiently understood. Here, nickel phthalocyanine (NiPc) is investigated, a benchmark CO 2 R catalyst, supported on CNTs. NiPc preferentially anchors at defect-sites on CNTs rather than adsorbing uniformly via π-π stacking is found, an observation validated by theoretical simulations. Notably, CNTs with the fewest defects, despite exhibiting non-uniform NiPc distribution, deliver the highest CO 2 R activity and CO selectivity. Operando X-ray absorption spectroscopy reveals that high defect densities induce D 4 h symmetry distortion of the NiPc macrocycle under cathodic bias, compromising catalyst integrity and CO 2 R performance. Guided by these insights, CNT defect density is optimized via thermal graphitization, yielding a NiPc/CNT composite with unprecedented selectivity (CO:H 2 > 16 100:1) and a turnover frequency of 1072 s⁻ 1 at −0.60 V versus RHE, switching off the competing hydrogen formation. Integrated into a 100 cm 2 zero-gap electrolyzer, the optimized catalyst sustains 50 A current with >95% CO selectivity at ≈3.5 V, outperforming state-of-the-art Ag-based systems. This work establishes CNT defect-engineering as an effective strategy for advancing molecular catalysts for CO 2 R electrolysis.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
H. Yu,C. Sun,Y. Xuan,K. Zhang,K. Chang
Photocatalytic carbon dioxide (CO 2 ) reduction to valuable chemicals (ethanol) is an ideal way to realize artificial photosynthesis. It is still extremely difficult to achieve the challenge for photocatalytic CO 2 reduction to multi-electronic products (C 2 H 5 OH). Here, we design the SrTiO 3 (La Cr)/Cu @ Ni/TiN (STO/Cu @ Ni/TiN) to realize the high efficiency of photocatalytic CO 2 reduction conversion into ethanol in the absence of sacrificial reagents. Furthermore, we use non-noble metallic materials such as Cu, Ni, and TiN to enhance the plasmonic effect for efficiently capturing solar full-spectrum energy instead of noble metals. Meanwhile, the TPD results show that Cu@Ni nanoparticles can enhance the chemical adsorption of CO 2 molecules. STO/Cu @ Ni/TiN exhibit an optimal ethanol evolution rate of 21.3 μmol/(h·g cat. ) and the ethanol selectivity of 79%, which is the highest value for photocatalytic CO 2 reduction to ethanol, among the best values of our knowledge. Furthermore, the pathway of ethanol is confirmed by density functional theory (DFT) calculations and the 13 C isotope experiment.
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ACS Nano
·
2021
·
IF 15.881
Zhiyi Wu,Chaoran Li,Zhao Li,Kai Feng,Mujin Cai,Dake Zhang,Shenghua Wang,Mingyu Chu,Chengcheng Zhang,Jiahui Shen,Zheng Huang,Yanling Xiao,Geoffrey A. Ozin,Xiaohong Zhang,Le He
The conversion of CO2 into fuels and feedstock chemicals via photothermal catalysis holds promise for efficient solar energy utilization to tackle the global energy shortage and climate change. Despite recent advances, it is of emerging interest to explore promising materials with excellent photothermal properties to boost the performance of photothermal CO2 catalysis. Here, we report the discovery of MXene materials as superior photothermal supports for metal nanoparticles. As a proof-of-concept study, we demonstrate that Nb2C and Ti3C2, two typical MXene materials, can enhance the photothermal effect and thus boost the photothermal catalytic activity of Ni nanoparticles. A record CO2 conversion rate of 8.50 mol·gNi–1·h–1 is achieved for Nb2C-nanosheet-supported Ni nanoparticles under intense illumination. Our study bridges the gap between photothermal MXene materials and photothermal CO2 catalysis toward more efficient solar-to-chemical energy conversions and stimulates the interest in MXene-supported metal nanoparticles for other heterogeneous catalytic reactions, particularly driven by sunlight.
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