CHEMICAL ENGINEERING SCIENCE
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2024
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IF 4.1
Youwei Yang,Mengjiao Zhang,Busha Assaba Fayisa,Ziheng Zhen,Ying Hu,Mei-Yan Wang,Shouying Huang,Yue Wang,Xinbin Ma
The selective hydrogenation of ethylene carbonate (EC) to produce methanol (MeOH) and ethylene glycol (EG) is a crucial route to achieve indirect and efficient utilization of CO 2 under mild reaction conditions. Nonetheless, due to the cyclic carbonate structure of EC, the intricate reaction network involved in the hydrogenation process has not been systematically reported yet. Here, a series of Cu/SiO 2 catalysts were designed to investigate the related reaction pathways. The catalytic evaluation results, coupled with thermodynamic calculations, reveal that there are several competitive side-reactions other than EC hydrogenation to MeOH and EG, including decarboxylation, hydrolysis and decarbonylation reactions to produce CO 2 and CO as byproducts. Moreover, the distribution of products is significantly influenced by evaluation conditions. Furthermore, by doping metal oxides to adjust the surface properties of Cu/SiO 2 catalyst, it is found that acidic sites could promote EC hydrolysis, whereas basic sites predominantly facilitate EC decarboxylation and decarbonylation reactions. Overall, a comprehensive reaction network of EC hydrogenation is systematically proposed to provide appropriate evaluation conditions and guidance for designing new catalysts to minimize unwanted side reactions, which is of great significance to enhance the indirect utilization of CO 2 .
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RESEARCH ON CHEMICAL INTERMEDIATES
·
2025
·Vol. 51
·期 4
·2071-2088
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IF 3.5
Wu Yilin,Li Yiping,Zhang Kai,Hu Jinhai,Yan Hong
Photocatalytic CO 2 reduction technology can use sunlight to convert CO 2 into fuel or chemical raw materials, slowdown the greenhouse effect and achieve sustainable development. Therefore, we have developed a series of high-quality carbon quantum dots using alkaline lignin (AL) as the core raw material and using high efficiency hydrothermal method. Ag-BiVO 4 composite was prepared by hydrothermal method. Then, the Ag-BiVO 4 -CQDs photocatalytic composite was prepared by constant temperature water bath method. The structure and morphology of the composites were characterized by X-ray diffraction, transmission electron microscope and X-ray photoelectron spectroscopy. Through optical and electrochemical tests, it can be seen that the composite has better interfacial charge transfer and electron transport ability. In the visible light catalytic CO 2 reduction reaction, Ag-BiVO 4 can selectively reduce CO 2 to CH 4 , and the CH 4 yield is greatly improved after Ag-BiVO 4 combines with CQDs. The 3 h CH 4 yield increased from 17.64 μmol/g to 97.82 μmol/g after reduction by adding 40 mL CQDs to Ag-BiVO 4 composite, which is 5.54 times that of Ag-BiVO 4 . The results showed that the introduced CQDs were uniformly attached to Ag-BiVO 4 . As an electron transport medium, CQDs can efficiently facilitate the transfer of photogenerated carriers, suppress the recombination of electron–hole pairs, and enhance the photocatalytic performance of Ag-BiVO 4 -CQDs for CO 2 reduction.
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JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY
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2025
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IF 1.9
M. L. Shao,M. J. Cheng,J. Gong,A. L. Chang,L. P. Fu,K. L. Liao,X. Q. Liu
Carbon dioxide (CO2) flooding is one of the efficacious channels to enhance oil recovery efficiency of low permeability reservoirs. However, CO2 gas channeling has seriously affected the development effect due to severe formation heterogeneity. Nanomaterials have good application prospects in plugging gas channeling, but the dispersibility in water limits the plugging effect. In this paper, a nanoparticle plugging agent with a core-shell architecture was synthesized via emulsion polymerization. The impacts of different elements such as grain diameter, temperature and salinity on the swelling characteristic of nanoparticles were studied respectively. Subsequently, the CO2 response property of nanoparticles was tested by uniformly injecting CO2. Finally, based on the calculation of molecular dynamics, the interaction between nanoparticles and water molecules was analyzed. The results showed that the CO2-responsive nanoparticles exhibit a lower swelling ratio (<5), and the residual resistance coefficient is 2.47, demonstrating a limited expansion property and superior plugging performance. The interaction between protonated nanoparticles and water molecules was stronger, resulting in enhanced hydrophilicity and responsive inflation of nanoparticles. The system has great potential application prospects for in-depth CO2 conformance control.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Xiaojiang Li,Xingqiao Zhang,Chengwei Zuo,Han Zhang,Zhenfu Jia
Cleaner recovery of petroleum hydrocarbons is a key process for waste oil and gas resources, especially oily waste solid. However, the direct recovery of petroleum hydrocarbons is difficult with deep eutectic solvents (DES) without other additives (such as water). In this work, ionic liquid-based DESs (ILs-DESs) with a controllable polarity were prepared for the sustainable recovery of petroleum hydrocarbons. Here, CO2-responsive ionic liquids were prepared by the neutralization reaction of 1,8-diazabicyclo[5.4.0]undec-7-ene and iminazole (Im), pyrazol (Py), or triazole (Tri). Then, the ILs-DESs were separately prepared by using ionic liquids as proton acceptors and straight-chain alcohols (carbon number = 4, 6, 8, 10, and 12) as proton donors. The polarity transformation of the ILs-DESs was regulated only by the introduction and removal of CO2, which was caused by the reversible transformation from ILs-DESs with a lower polarity to alkyl carbonate and carbamate with higher polarity upon CO2. Because of the polarity changes, the simulated oil (such as n-dodecane or diesel oil) was mixed with ILs-DESs, and the samples were directly separated by introducing CO2. Finally, a sustainable process for treating oil sands and oily sludge by using ILs-DESs was developed, where the ILs-DESs were also reused more than twice. This implies that a sustainable approach for petroleum hydrocarbon recovery was realized by using DESs.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Mengchen Wu,Yang Yang,Jing Zhao,Rui Liu
In CO 2 electroreduction, mutative intermediates and the challenging C C coupling necessitate the spatial interplay between active sites and through dynamically optimizing configurations. Herein, we anchor ethylenediaminetetraacetic acid (EDTA)-bonded Cu x+ /Bi 3+ pair within UiO-66 for a spontaneous spatial-optimizing CO 2 -to-C 2 H 4 electroreduction. Ab initio molecular dynamic (AIMD) simulation visualizes that such metal pair adaptively interacts with intermediates. Density functional theory (DFT) elicits the componential synergy, in which an upshift d-band of Cu activates CO 2 being protonated into *COOH while Bi site stabilizes oxygenated dimers for deep hydrogenation. The dynamic feature of such pair affords large freedom for sorption and migration of various intermediates, which consequently bestows UiO-66-EDTA/CuBi a maximal FE C 2 H 4 of 47 % and a total current density over 100 mA cm −2 in the flow cell.
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CATALYSIS COMMUNICATIONS
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2024
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IF 3.4
Zhi-Gang Hu,Lichun Li,Shui-Bao Yu,Zhengfei Chen,Jian-Quan Weng
Several tertiary amine solutions with different structures were tested in the integrated CO 2 capture and hydrogenation process in the presence of heterogeneous Pd/NAC catalysts. The tertiary amines of 3-dimethylamino-1,2-propanediol (3DMA-1,2-PD) and 3-diethylamino-1,2-propanedio (3DEA-1,2-PD) with high CO 2 absorption capacity and high formate yield were selected as suitable candidates as CO 2 capture and hydrogenation solvents. Under mild reaction conditions, a high formate yield of 68% was achieved when using 1 M 3DMA-1,2-PD solution with CO 2 loading of 0.5 mol amine/mol CO 2 . In addition, the physico-chemical properties of the Pd/NAC catalysts were examined and the reaction mechanism of CO 2 absorption and hydrogenation in the presence of Pd/NAC was proposed.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-15
·
IF 15.7
Cai Zhongjie,Liu Hongwei,Dai Jiajun,Li Bao,Yang Liming,Wang Jingyu,Zhu Huaiyong
Overall artificial photosynthesis, as a promising approach for sunlight-driven CO 2 recycling, requires photocatalysts with efficient light adsorption and separate active sites for coupling with H 2 O oxidation. Here we show a In-based metal–organic framework (MOF) heterostructure, i.e., In-porphyrin (In-TCPP) nanosheets enveloping an In-NH 2 -MIL-68 (M68N) core, via a facile one-pot synthesis that utilises competitive nucleation and growth of two organic linkers with In nodes. The coherent interfaces of the core@shell MOFs assure the structural stability of heterostructure, which will function as heterojunctions to facilitate the efficient transfer of photogenerated charge for overall photosynthesis. The In-TCPP shell in MOFs heterostructure improves CO 2 adsorption capabilities and visible light absorption to enhance the photocatalytic CO 2 reduction. Simultaneously, In-O sites in M68N core efficiently catalyze H 2 O oxidation, achieving high yields of HCOOH (397.5 μmol g −1 h −1 ) and H 2 O 2 (321.2 μmol g −1 h −1 ) under focused sunlight irradiation. The superior performance of this heterostructure in overall photosynthesis, coupled with its straightforward synthesis, shows great potential for mitigating carbon emissions and producing valuable chemicals using solar energy.
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ACS Catalysis
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2024
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IF 11.3
Yueqi Feng,Jiaomei Xiao,Yiyi Qiu,Jianlin Huang
Precise control and understanding of surface changes in indium (In)-based catalysts during the electrocatalytic CO2 reduction reaction (CO2RR) process are challenging. This study presents a series of surface-reconstructed In2O3–Bi electrocatalysts, created by doping mesoporous In2O3 nanocubes with bismuth (Bi). This doping introduces abundant bimetallic In–Bi sites at the crystal–amorphous interfaces, enhancing the CO2-to-formate conversion selectivity. Bi atoms accelerate the surface reconstruction of In2O3, reduce the charge density around In atoms, and promote partial amorphization. In situ X-ray diffraction (XRD) and Fourier-transform infrared spectroscopy (FT-IR) measurements and density functional theory (DFT) calculations show that the bimetallic In–Bi sites lower the energy barrier for the HCOOH* intermediate, enhance H2O dissociation, and inhibit the hydrogen evolution reaction (HER). The surface-reconstructed In1.8Bi0.2O3 electrocatalyst demonstrates a Faradaic efficiency (FE) of 92.6% and a partial current density of −28.5 mA·cm–2 and operates stably for 110 h in a H-type cell. In a flow cell, it achieves an FE of formate (FEformate) of 97.6% at −1.4 VRHE and maintains above 94% FEformate over a potential window of 800 mV (from −1.0 to −1.8 V vs RHE). This study offers an effective approach for designing high-performance electrocatalysts for the CO2RR based on surface reconstruction.
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AICHE JOURNAL
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2024
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IF 3.5
Xueqi Sun,Shaojuan Zeng,Guilin Li,Yinge Bai,Minghua Shang,Jian Zhang,Xiangping Zhang
The selective separation of CO 2 from CH 4 -containing gases is crucial to produce clean energy gases. In this study, triazole anion-functionalized ionic liquids (TAFILs) were designed by combining low molecular weight cations with triazole anions containing N electronegative site and further mixed with physical solvents to form physicochemical absorbents. The results indicated that [Cho][Triz]/TMS (80 wt%/20 wt%) not only absorbs 0.125 g CO 2 /g absorbent equal to that of 30 wt% MEA solution at 40°C and 1 bar, but also has low enthalpy of −35.76 kJ/mol less than half of 30 wt% MEA solution. Simultaneously, a super high CO 2 /CH 4 selectivity of 191.0, higher than most of the reported absorbents, is obtained for [Cho][Triz]/TMS solvents. Such great performance of CO 2 separation was attributed to relatively weak chemical and physical interaction between CO 2 and TAFIL binary absorbents. This study may provide novel promising ionic liquid absorbents for CO 2 capture applications from clean energy gases.
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Materials Chemistry Frontiers
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2025
·
IF 6.4
Yapeng Dong,Yuning Liang,Bo Gao,Qun Xu
Exploring advanced technology to obtain quantum materials presenting novel and unexpected electronic states upon proper manipulation is an important research endeavor. Usually, plastic deformation can lead to some amount of disruption that can result in new physical phenomena and fascinating structures. However, how to realize efficient plasticization and manipulation to obtain irreversible variation in such materials, especially those presenting quantum material behavior, is a great challenge. Herein, we show that upon plastic deformation induced by supercritical CO2 (SC CO2) on SrZrO3, typically at a pressure of 16 MPa, SrZrO3 experiences a transition from a bulk material to a two-dimensional (2D) structure. More importantly, it can be observed that the octahedral rotation of ZrO6 is suppressed. Furthermore, plastic deformation frequently induces magnetism in SrZrO3. Via polarization characterization, SrZrO3 displays multiferroic characteristics, exhibiting a considerable enhancement in the saturation magnetisation strength and polarization strength. At room temperature, SrZrO3 exhibits a saturated magnetisation of 0.1280 emu g−1, accompanied by a polarization of 0.27 μC cm−2. Therefore, this work demonstrates that plastically deformed SrTiO3 induced by SC CO2 can successfully transition into a quantum multiferroic material. These results establish a new method toward plastic deformation for the manipulation of the electronic properties of quantum materials.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-13
·
IF 14.7
Zou Yunjie,Mao Chengliang,Xu Mingkai,Xing Chao,Wang Ruizhao,Ozin Geoffrey A.,Ling Lan
Gas-phase heterogeneous catalytic CO 2 hydrogenation to commodity chemicals and fuels via surface frustrated Lewis pairs is a growing focus of scientific and technological interest. Traditional gas-phase heterogeneous surface frustrated Lewis pair catalysts primarily involve metal oxide-hydroxides (MOH•••M). An avenue to improve the process performance metrics lies in replacing the Lewis base MOH with a stronger alternative; an intriguing example being the amine MNH 2 in metal nitrides. This study establishes a proof-of-concept that an amine-type photoactive surface frustrated Lewis pair (MNH 2 •••M) can be constructed in titanium nitride (TiN x O y ) when integrated with a nanoscale platinum spillover co-catalyst. This surface frustrated Lewis pair, comprising Ti-NH 2 as the Lewis base and low-valent Ti as the Lewis acid, facilitates the gas-phase light-assisted heterogeneous reverse water-gas shift reaction. The reaction proceeds via a surface-active carbamate intermediate, Ti-(H 2 N-COO)-Ti, whereby the synergism of Lewis acidic and Lewis basic sites endows it with superior performance indicators compared to TiN x O y alone, as well as conventional platinum supported metal oxides.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Mazhar Khan,Zeeshan Akmal,Muhammad Mubashir Khan,Muhammad Tayyab,Seemal Mansoor,Muhammad Adnan Zeb,Amir Zeeshan,Ziwei Ye,Jinlong Zhang,Shiqun Wu,Lingzhi Wang
Metal-organic framework (MOF) based heterojunctions offer a promising strategy for CO 2 photoreduction, contributing to carbon neutrality and environmental remediation. However, the precise design and control of these heterostructures remain critical challenges. Herein, we report the precise construction of a heterostructure by integrating 2D ZnIn 2 S 4 nanosheets with NH 2 -MIL-125(Ti) for efficient CO 2 photoreduction in a sacrificial agent-free environment. A comprehensive investigation demonstrates robust interfacial interactions and work function differences between NH 2 -MIL-125(Ti) and ZnIn 2 S 4 , facilitating the formation of an interfacial electric field and enabling the construction of an S-scheme heterojunction. The directional migration of photogenerated charge carriers effectively suppresses their recombination, retaining the strong oxidative and reductive potential of the heterostructure components. In-situ infrared spectroscopy provides concrete evidence that the S-scheme heterojunction significantly enhances the formation of key intermediates, which are crucial for CO generation. The optimized NMT-5@ZIS achieves a CO yield of 17.30 umol g -1 h −1 without sacrificial agents, representing 8.6 and 6.6-fold improvements over pristine NH 2 -MIL-125(Ti) and ZnIn 2 S 4 , respectively. This work bestows an innovative insight into the construction of MOF-based S-scheme heterojunctions, opening new avenues for practical applications in energy storage and photocatalysis.
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