NEW JOURNAL OF CHEMISTRY
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2024
·Vol. 48
·期 17
·7982-7989
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IF 2.7
Naitian Zhang,Yuehui Li,Wenzhe Shang,Wei Liu,Xusheng Cheng,Suchan Song,Xuedan Song,Yantao Shi,Ce Hao
In this paper, we investigated the role of excited-state hydrogen bonding in the photocatalytic carbon dioxide reduction reaction (CO2RR) utilizing Rose Bengal as a catalyst, through a combined experimental and theoretical approach. Experiments validated the successful conversion of CO2 to CO in a homogeneous aqueous solution system under light irradiation, without additional photosensitizers or sacrificial agents. Theoretically, the DFT/TDDFT calculations modeled the catalyst-reactants as a hydrogen-bonded complex (HBC), understanding the energy, hydrogen, and electron transfer mechanisms induced by excited-state hydrogen bonding. Combining the photophysical and photochemical insights revealed the complete catalytic cycle, identifying the water oxidation process as the rate-limiting step in the entire photocatalytic CO2RR process. Experimental and computational results provide molecular-level insights into the structure–activity relationships. This work enhances comprehension of the pivotal role of excited-state hydrogen bonding and holds significant reference value for enhancing the conversion efficiency in the photocatalytic CO2RR.
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高影响因子
ENERGY
·
2025
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IF 9.4
Kefei Li,Yue Wu,Yiming Bai,Hai Yan,Yiming Wang,Yuzhe Guan,Liang Li,Guicheng Liu
Reducing the energy consumption of CO 2 regeneration is crucial for enhancing the economic feasibility of CO 2 capture processes. While most studies have focused on developing novel absorbents, the influence of operating parameters on gas-liquid mass transfer behavior and their subsequent impact on energy consumption has received limited attention. This study experimentally investigates the regeneration heat duty (Q reg ) for CO 2 desorption from a 1-(Dimethylamino)-2-propanol (1DMA2P)/2-Methylaminoethanol (MAE) aqueous blend in a lab-scale stripper equipped with high-efficiency Sulzer DX structured packing. The effects of key operating parameters, including rich CO 2 loading, lean CO 2 loading, solution flow rate, amine concentration, and synergistic parameters (Δ α × L and C × L ), on Q reg were systematically analyzed. The experimental results showed that all these factors greatly influenced Q reg . For example, the Q reg decreases as the lean CO 2 loading (α lean ) , rich CO 2 loading (α rich ) , and 1DMA2P/MAE concentration (C) increase, indicating that the Q reg can be reduced by optimizing these operating parameters. Additionally, compared with MEA, 1DMA2P/MAE reduces energy consumption by 51.5 % and decreases the stripper height by 35 %. This study underscores the critical role of operating parameters in reducing CO 2 regeneration energy consumption. The findings provide valuable insights into optimizing stripper performance and demonstrate the advantages of the 1DMA2P/MAE blend as an energy-efficient alternative to MEA-based solvents in industrial CO 2 capture applications.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Lei Xiong,Xianbiao Fu,Jun Zhang,Shuang Liu,Shanshan Li,Shaojie Lu,Dong Wang,Qin Yue
Cu shows unique characteristics for electrochemical CO 2 reduction reaction (CO 2 RR) to hydrocarbons and oxygenates due to the moderate adsorption energy of the key intermediate *CO. However, it remains a challenge to selectively control CO 2 RR towards C 1 (e.g., CH 4 ) or C 2+ (e.g., C 2 H 4 and C 2 H 5 OH) through simple interface engineering. Herein, a series of inverse catalysts, composed of CeO 2 nanoparticles over Cu substrate (Cu-CeO 2 -x), are subtly designed to tackle the issues. It is verified CeO 2 decoration induces highly active Cu/CeO 2 interfacial sites that enhance the adsorption and conversion of CO 2 and *CO intermediates into C 2+ or CH 4 , while the Cu sites are conducive to *CO generation. With the increase of CeO 2 deposition, the C 2+ and CH 4 selectivity present a volcano-type and increasing tendency with maximum faradic efficiency of 62.6% and 51.3%, respectively. In-situ infrared spectroscopy and theoretical calculations reveal that moderate CeO 2 loading allows the Cu/CeO 2 interfacial sites to cooperate efficiently with the Cu sites to promote the coupling of *CO/*CHO intermediates, thus enhancing the C 2+ selectivity. In contrast, excessive CeO 2 loading suppresses the C─C coupling but boosts unilaterally the hydrogenation, thus promoting the CH 4 production. This work provides effective strategies to regulate the CO 2 RR selectivity by modulating metal/oxide interfaces.
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RSC Advances
·
2024
·Vol. 14
·期 10
·6502-6507
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IF 3.9
Jiaqi Wang,Kaihong Liu,Jingjing Zhao,Xiuping Li,Bolin Yin,Bo Jiang,Hexing Li
Direct CO2 hydrogenation to value-added chemicals is a promising path toward realizing the “carbon-neutral” goal. However, controlling the selectivity of CO2 hydrogenation toward desired products (e.g., CO and CH4) using non-precious metal-based catalysts is important but challenging. It is imperative to explore catalysts with high activity and stability. Herein, boron-doped cobalt nanoparticles supported on H-ZSM-5 were devised for CO2 hydrogenation to produce CO in a gas–solid flow system. Our results demonstrate that boron doping not only increases the CO2 adsorption capability of the catalyst but also optimizes the electronic state of Co for CO desorption during hydrogenation process. As a result, the boron-doped cobalt catalysts displayed an enhanced CO selectivity of 94.5% and a CO2 conversion rate of 45.6%, which is much higher than that of Co-ZSM-5 without boron doping. This study shows that the strategic design of metal borides is important for controlling the selectivity of desired products in the CO2 hydrogenation reaction.
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Jin Liu,Shiyong Sun,Rui Lv,Sen Lin,Yevgeny A. Golubev,Ke Wang,Rui Cao,Yifan Zeng
The unparalleled catalytic activity of carbonic anhydrases (CAs) towards CO 2 hydrolysis can potentially contribute to carbon capture, utilization, and storage technology aimed at global decarbonization; however, the high cost and low stability of CAs significantly limit their practical applications. Recently, the development of robust and effective nanozymes with CA-mimicking activity has been proposed as a promising solution to this challenge. Herein, a novel zinc-based organophyllosilicate (ZnAC) nanozyme with CA-like catalytic activity was synthesized by a facile one-pot sol–gel method for the first time, leading to a Zn-O coordination structure that mimicked the catalytic center fragments of natural CAs, with surface amino groups acting as the affinity sites and proton shuttles. The synergistic effect of the two components on the open surface of the layered structure resulted in excellent CA-like activity with a Michaelis–Menten constant (K m ) of 4.071 mM, maximum velocity (V max ) of 0.220 mM/s, and turnover number (k cat ) of 11.213 /s at 25 °C and pH=7.5, which were superior to those of most previously reported CA-like nanozymes. The catalytic performance of ZnAC significantly improved with increasing pH and temperature; furthermore, ZnAC exhibited excellent stability, maintaining high catalytic activity after the exposure to extreme temperatures or pH values, eight reaction cycles, and 30 d of storage. Additionally, ZnAC significantly increased the rate of CO 2 hydration and the extent of CO 2 mineralization and precipitation. This work proposes a new strategy for designing and constructing efficient CA-like nanozymes, providing valuable insights into the structure–activity relationship and new perspectives for the implementation of CO 2 fixation.
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APPLIED ENERGY
·
2024
·
IF 10.1
Heng Pan,Yuhao Zhao,Feiyu He,Liya Zhu,Zhaolu Wang,Yihang Li,Youjun Lu
Solar CO 2 splitting via a two-step thermochemical cycle (TSTC) has emerged as a promising technology for solar fuel production. However, the extreme reduction temperature ( T red ) required to achieve optimal CO yields poses challenges in reactor design, operation, and solar-to-fuel energy efficiency. In this study, a two-step electro-thermochemical cycle (TSEC) for CO 2 splitting into CO using a solid oxide electrochemical cell (SOEC) is presented with the objective of reducing T red and improving solar-to-fuel energy efficiency. The investigations reveal that TSEC exhibits the capability to decrease T red from 1500 °C to 1000 °C, while simultaneously maintaining a substantial CO yield of 550 μmol/g. Moreover, the efficiency analysis demonstrates that TSEC achieves a superior solar-to-fuel energy efficiency of 20.4 %, outperforming 4.1 % of conventional TSTC. In sum, this study demonstrates a novel approach to solar fuel production, enabling high and stable CO 2 -to-CO conversion at moderate temperatures while maintaining high energy efficiency.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jie Qi,Jian Lan,Shaoyang Liu,Li Tong,Yuzhe Li,Na Wang,Zheng Zhang,Hongsheng Lu
One of the challenge in the remediation of contaminated soil by solvent washing is the retrieval of total petroleum hydrocarbons (TPH) and solvents. Herein, a CO 2 switchable hydrophobic low temperature transition mixture ([DPA][EL]) composed of ethyl lactate (EL) and dipropylamine (DPA) is proposed, accompanied by a proof-of-concept for contaminated soil washing. The path and energy of hydrogen bond interactions in [DPA][EL] were revealed by the quantum chemical calculation using the quantum theory of atoms in molecule. [DPA][EL] achieved a thorough CO 2 -induced polarity and hydrophobicity transition undergoing an incomplete CO 2 absorption that results in the partial formation of carbonate and carbamate. [DPA][EL] was regenerated after the removal of CO 2 by heating at 85 °C for 2 min. Thanks to this peculiarity, the time required for hydrophobicity transition was 197 times shorter than that of the typical CO 2 switchable hydrophobic solvent, N,N -dimethylcyclohexylamine. The polarity of [DPA][EL], quantified by the normalized polarity energy, increased by 346.69 % after the introduction of CO 2 because of the synergistic effect of water. This ultra-sensitive transition behavior intensified the CO 2 -induced separation of oily compounds, e.g., kerosene and crude oil. The conceptual usage of [DPA][EL] in the contaminated soil washing was demonstrated. The TPH content of contaminated soil decrease from 8.27 % to 0.31 % by [DPA][EL] washing through tailoring the molar ratio of DPA to EL in [DPA][EL], temperature, and [DPA][EL] to contaminated soil ratio (L/S, mL/g). [DPA][EL] whose composition possesses different polarities compensated for the poor solubility of single solvents towards TPH, thereby improving the washing efficiency of contaminated soil. Afterwards, TPH was separated upon triggered by CO 2 /water in 2 min, and 91.33 % of [DPA][EL] was subsequently regenerated at 85 °C in 2 min.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
·
IF 5.8
Jihai Zhao,Qi Wang,Yaowen Wang,Xinbo Li,Chang Liu,Taotao Huang,Liping Li,Guangshe Li
The spin state of transition metal ions, specifically controlled by the electrons in antibonding orbital, is recognized as a descriptor for heterogeneous catalysts. However, the influence of spin state on the adsorption of CO molecular with two electrons in the highest occupied molecular orbital, has been overlooked. In this work, the Co 2+ spin states in multicomponent rock-salt oxides are regulated by increasing configurational entropy, demonstrating the impact of Co 2+ spin states on CO adsorption. The CO catalytic oxidation activity of as-synthesized rock-salt oxides exhibits a volcano-shaped relationship with the ratio of Co 2+ in high spin state to Co 2+ in low spin state. Mg 0.33 Co 0.33 Ni 0.33 O with this spin state ratio of 7.5 has the largest negative adsorption energy to CO molecular and exhibits the best catalytic activity. The findings on the relationship between the spin state of transition metal ions and reactant adsorption can contribute to the understanding of catalytic activity at the electronic level.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Jiping Shi,Liuqing Hua,Lu Ruan,Xingjian Zhang,Zhengdao Li,Fengyun Su,Xin Li,Haiquan Xie,Yong Zhou
The ZnIn 2 S 4 nanosheets were successfully synthesized on the surface of compacted stainless steel mesh using a simple solvothermal method, and further modified with Cu x O nanoparticles to form ZnIn 2 S 4 /Cu x O heterojunction photocatalyst via a wet chemistry approach. These photocatalysts were then utilized for photothermal catalytic CO 2 reduction under full spectrum solar light. The experimental results demonstrated that the deposition of the photocatalyst on the flexible substrate effectively prevented the aggregation of ZnIn 2 S 4 nanosheets. The incorporation of Cu x O nanoparticles enhanced the specific surface area of the photocatalyst, and created a Z-scheme heterojunction with ZnIn 2 S 4 to improve the utilization efficiency of photogenerated electrons. It was noteworthy that the dark red Cu x O exhibited a full spectrum response and excellent photothermal effect, thereby facilitating carrier migration and reducing CO 2 catalytic reaction barriers. Consequently, the optimized ZnIn 2 S 4 /Cu x O exhibited significantly enhanced CO 2 to CO yield of 1515.8 μmol m -2 h −1 and CH 4 yield of 1579.4 μmol m -2 h −1 , which was about 7.5 and 7.6 times higher than those achieved by pure ZnIn 2 S 4 , respectively. Furthermore, this study provided detailed insights into the mechanism of photocatalytic CO 2 reduction over composite material as well as valuable guidance for designing immobilized photocatalysts with high activity for CO 2 reduction.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhipeng Chen,Tao Wang,Chao Li,Mengxiang Fang,Wei Chen,Ximing Hu,Yan Shao,Zhihao Liu,Wei Zhang,Li Zhang,Wenyang Fan,Shaojuan Zeng
Lower regeneration energy and superior cyclic capacity have enabled biphasic absorbents great potential in the area of flue gas CO 2 capture. The liquid film mass transfer coefficient(k L ) is a vital parameter in the development of absorbents with efficient CO 2 absorption mass transfer performance, while the phase separation behavior of biphasic solutions could be an essential factor for the absorption mass transfer and the stability of absorber. However, systemic kinetic research towards biphasic absorbents, especially the impact of phase separation behavior, is limited. In this study, a typical amide-based biphasic absorbent diethylenetriamine(DETA)/diethanolamine(DEA)/N, N-dimethylacetamide(DMAC) which has achieved great reduction in regeneration energy, was selected as the subject of kinetic investigation in a wetted wall column. The CO 2 overall mass transfer coefficient(K G ) of DETA/DEA/DMAC exceeded other biphasic solvents, blended amine solution, and 40% K 2 CO 3 solution, with 3 times that of 40% K 2 CO 3 solution. Moreover, various operational conditions including absorption temperature, gas flow rate, and water content of solution were taken into account to build a multiple-condition kinetic mechanism to offer guidance for biphasic absorbents. Furthermore, phase separation behavior was revealed as the main blame for the deterioration in the liquid film chemical mass transfer process of biphasic solvents in the CO 2 absorption process, resulting in the k L of DETA/DEA/DMAC before phase separation decreased by 75.3% at the phase separation stage. Therefore, it is crucial to ensure that the CO 2 loading of the solution entering absorber is lower than the phase separation point in applications. After phase separation, DETA/DEA/DMAC split into the organic and aqueous phases, the k L of the aqueous phase gradually exceeded that of the organic phase as CO 2 loading increased for its higher chemical enhancement factor(E).
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Xiaohong Chen,Wei Zou,Shengke Liang,Hong Wang,Chen Zhang
Adsorbent materials with high adsorption efficiency, good processing stability, and high adsorption rate, are crucial for carbon capture, utilization and storage (CCUS) technology. In this paper, a novel polyethyleneimine (PEI)-embedded porous adsorbent with high amine-content matrix was one-step prepared successfully by a unique high internal phase emulsion (HIPE) polymerization. Firstly, the amphiphilic polyethyleneimine-based carbon nanotubes (CNT-PEI) was synthesized and applied as a Pickering emulsifier, and the interfacial tension was analyzed by a multi-functional tensiometer. Secondly, a large amount of divinylbenzene (DVB) was introduced into the continuous phase of HIPE, and then some mesopores were generated in the framework of the macro-porous polymer, which indicated by specific surface and pore size analyzer and scanning electron microscope (SEM), respectively. Finally, the additional PEI was added into the dispersed phase of HIPE. In such unique HIPE template, PEI was penetrated into the framework and then the porous polymer with high amine-content matrix was achieved. The morphology, the surface element content and the CO 2 adsorption capacity of the obtained porous polymer were characterized by SEM, energy dispersive spectrometry (EDS), and the gas sorption analyzer. When the obtained porous polymer was applied as CO 2 adsorbent, the better comprehensive adsorption performance, including high CO 2 adsorption capacity of 2.87 mmol/g, fast adsorption kinetics, the isosteric heat of adsorption (Q st ) range of 65–68 kJ/mol, exceptional CO 2 /N 2 selectivity with a separation factor up to 118, and stable adsorption–desorption cycles, was exhibited. The superior CO 2 adsorption capacity and adsorption kinetics make it a promising candidate in practical CO 2 adsorption application.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2024
·
IF 2.7
Jiaqi Huang,Jian Zhang,Xiujun Wang,Bo Huang,Zhao Hua,Shenwen Fang
Improving the stability of CO 2 foam is a core concern in CO 2 foam flooding oil recovery technology. Using hydrophobic nano-SiO 2 to enhance the stability of CO 2 foam is a common approach, but hydrophobic nano-SiO 2 faces challenges, such as easy aggregation, difficult dispersion, and performance needs to improve. In this article, a novel dispersion of styrene-phenylamine monomer copolymer (PSSN) nanosphere with primary amine groups on the surface was synthesized. The synthesis conditions of PSSN were optimized, and its performance for stabilizing CO 2 foam was evaluated. The experimental results demonstrated that PSSN had better performance for stabilizing CO 2 foam than that of hydrophobic nano-SiO 2 when using cocamidopropyl betaine (CAB) as the foaming agent. With the CAB concentration of 4000 mg/L and PSSN concentration of 100 mg/L in the brine having salinity of 8460 mg/L, the half-life of CO 2 foam at 90°C was 131 min, which was 43 min longer than that stabilized by hydrophobic nano-SiO 2 under the same conditions. This is for the first time that polystyrene microspheres with amine groups on the surface was used to stabilize CO 2 foam. The study provides a new nanoparticle option for stabilizing CO 2 foam.
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