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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Molecular Catalysis
·
2024
·
IF 3.9
Pengcheng Wang,Qingqing Jiang,XingYu Li,Xuedong Wang,Juncheng Hu
Generally, researchers focus on the regulation of metal sites rather than surrounding nonmetals in photothermal CO 2 hydrogenation reaction. Herein, concerning the role of non-metallic N species, a series of Co/NC-T catalysts have been fabricated via high-temperature pyrolysis of Zeolitic Imidazolate Frameworks-67. The CO 2 conversion rate shows a consistent tendency with the ratio of graphitized-N species while the product selectivity is closely related to the coordination state of Co-N x species. Co/NC-800 catalyst achieves high CO 2 conversion rate of 758 mmol g cat -1 h -1 with CH 4 selectivity of 99.6 %. After adding extra graphitized-N species, the CO 2 conversion rate could further enhance to 80.2 % for N-Co/NC-2. The role of N species in photothermal CO 2 hydrogenation reaction has been investigated in details, providing new insights for the design of metal organic frameworks derived metal/N-doped carbon catalysts.
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MACROMOLECULAR CHEMISTRY AND PHYSICS
·
2025
·
IF 2.7
Siriguleng Bao,Yong Sheng Bao,Agula Bao
Lignin has a high carbon content, but the production of porous carbon materials from it is challenging because of its complex structure and stable physicochemical properties. In this study, nitrogen-doped porous carbon materials are prepared by impregnating lignin with urea, using potassium hydroxide (KOH) as an activator. The physicochemical properties of the samples are investigated using various characterization methods. The results showed that the CO 2 adsorption capacity of the sample LUN-10-7, which has a urea solution concentration of 10% and an immersion time of 7 days, is 3.80 mmol g −1 at 1 bar and 298 K. The characterization results indicated that the abundant pore structure and excellent surface chemistry enhanced the sample's CO 2 adsorption performance. Additionally, the sample demonstrated high CO 2 /N 2 selectivity and cyclic stability, making it suitable for practical applications as an adsorbent.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
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 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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ADVANCED MATERIALS
·
2025
·
IF 26.8
Cunbao Huo,Shuwang Wu,Rongjiang Zhang,Zhiqiang Wu,Xiaoyong Tian,Lei Tan,Kexin Li,Yao Yang,Baojie Wang,Zhun Hu,Lingling Wu,Dichen Li
Conventional packed-bed catalysts suffer from single-scale porosity, insufficient mechanical strength, and suboptimal mass transfer efficiency. Inspired by the fractal structure of the lung bronchi, a design and 3D printing method for gradient meta-structural catalysts is proposed by integrating synthesized LaFe 0.5 Ni 0.5 O 3 (LFN) perovskite with pseudo-boehmite, achieving ultralow pressure drop and high catalytic efficiency. Computational fluid dynamics and reaction simulations guide the design of uniform and gradient-structured catalysts with hierarchical woodpile channels (0.5–3 mm). Compared with homogeneous catalysts, the gradient design theoretically exhibits 1.5-fold and 1.1-fold increases in flow velocity and hydrogen production, respectively. Meta-structural catalysts are fabricated with gradient multi-peak pore distribution (9.32 nm, 103.75 nm) by regionally modulating unit cell sizes and LFN content (11–35%) combined with the dehydroxylation of pseudo-boehmite. 3D-printed perovskite catalysts demonstrate a 78.7-fold increase in specific surface area (102.26 m 2 g −1 ) and compressive strength of 8.48 MPa. In dry reforming of methane (DRM) tests, it achieves 82.13% CH 4 conversion, and 9.69 mmol g −1 syngas yield, outperforming conventional powder-packed beds by 10% efficiency. This study achieves mass transfer and catalytic performance coupling by tuning gradient hierarchical pores and tailoring flow dynamics, offering a paradigm for robust, high-efficiency catalyst design across diverse applications.
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PubMed
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CHEMICAL ENGINEERING JOURNAL
·
2024
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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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NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 17
·7982-7989
·
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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Journal of the American Chemical Society
·
2025
·
IF 15.6
Hang Zhang,Zhiwen Jiang,Changjiang Hu,Pengfei Zheng,Jun Ma
The hydro/dicarboxylation of ethylene (C2H4) feedstock with CO2 to produce high-value carboxylic acids is an industrially relevant yet challenging reaction due to their extremely low reactivities. Herein, we present an effective strategy to synthesize propionic acid and succinic acid from a mixture of CO2 and C2H4 catalyzed by high-energy water radiolysis. The process involves the generation of CO2 radical anions via the barrierless attachment of hydrated electrons to CO2, facilitating an ambient, continuous carboxylation of C2H4 with an efficiency of 81.4%. Utilizing easily available electron beam irradiation, we achieved a combined production rate of 0.34 mmol L–1 min–1 for carboxylic acids, which is unattainable by the existing methods. Notably, product selectivity between hydro- and dicarboxylation was dose-rate/beam intensity-dependent: high-dose-rate irradiation favored succinic acid formation with a proportional yield of up to 65.4%, while milder conditions resulted in an 85.1% yield of propionic acid. We suggested that the simplicity and efficiency of the present carboxylation approach promote circular carbon in the sustainable chemical industry.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
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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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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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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Jiayue Yu,Yang Zheng,Binxin Lv,Aiming Huang,Junjun Zhang,Zizi Wang,Yifan Zhang,Yang Wu,Yanan Zhou,Yong Wang,Wen Luo
Covalent organic frameworks (COFs), with their unique structures, have gained attention in CO 2 reduction (CO 2 RR) and are often combined with metal active sites to enhance performance. However, the weak interactions between COFs and metals create ambiguity about their actual states under reaction conditions, hindering the design of high-performance catalysts. Understanding these interactions is therefore essential for the rational development of advanced CO 2 RR electrocatalysts. Herein, a TpBpy COF, synthesized from 2,4,6-triformylphloroglucinol (Tp) and 5,5′-diamino-2,2′-bipyridine (Bpy), was coordinated with copper acetate to serve as a model catalytic system for understanding the structural evolution of TpBpy-Cu during CO 2 RR and the corresponding impact on the catalytic performance. A selectivity shift from CO to multi-carbon products was observed with increasing Cu content and reaction time. By combining ex situ characterization techniques with in situ infrared and Raman spectroscopy, the reduction of TpBpy-Cu to metallic Cu particles was revealed. Density functional theory calculations further demonstrated that metallic Cu surfaces of the resulting Cu particles played a key role in lowering the C-C coupling free energy change, facilitating the production of multi-carbon products. This work provides fundamental insights into the application of copper-based COF composite catalysts in electrocatalytic CO 2 RR and offers valuable guidance for the design of more efficient Cu-COF composite catalysts.
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