Frontiers of Chemical Science and Engineering

ISSN 2095-0179

ISSN 2095-0187(Online)

CN 11-5981/TQ

邮发代号 80-969

2019 Impact Factor: 3.552

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Recent progress in photocatalytic NAD(P)H regeneration for photocatalytic-enzymatic-coupling system
Wei Lan, Maodi Wang, Huicong Dai, Qihua Yang
Frontiers of Chemical Science and Engineering    2024, 18 (4): 37-null.   https://doi.org/10.1007/s11705-024-2398-0
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The enzymatic redox reactions in natural photosynthesis rely much on the participation of cofactors, with reduced nicotinamide adenine dinucleotide/nicotinamide adenine dinucleotide phosphate (NADH/NADPH) or their oxidized form (NAD+/NADP+) as an important redox power. The photocatalytic regeneration of expensive and unstable NADH/NADPH in vitro is an important process in enzymatic reduction and has attracted much research attention. Though different types of photocatalysts have been developed for photocatalytic NADH/NADPH regeneration, the efficiency is still relatively low. To elucidate the key factors affecting the performance of photocatalytic NADH/NADPH regeneration is helpful to rationally design the photocatalyst and improve the photocatalytic efficiency. In this paper, we overview the recent progress in photocatalytic NADH/NADPH regeneration with the focus on the strategies to improve the visible light adsorption, the charge separation and migration efficiency, as well as the surface reaction, which jointly determine the overall photocatalytic regeneration efficiency. The potential development of photocatalytic NADH/NADPH regeneration and photocatalytic-enzymatic-coupling system is prospected finally.

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Insight into the selective separation of CO2 from biomass pyrolysis gas over metal-incorporated nitrogen-doped carbon materials: a first-principles study
Li Zhao, Xinru Liu, Zihao Ye, Bin Hu, Haoyu Wang, Ji Liu, Bing Zhang, Qiang Lu
Frontiers of Chemical Science and Engineering    2024, 18 (3): 25-null.   https://doi.org/10.1007/s11705-024-2388-2
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The composition of biomass pyrolysis gas is complex, and the selective separation of its components is crucial for its further utilization. Metal-incorporated nitrogen-doped materials exhibit enormous potential, whereas the relevant adsorption mechanism is still unclear. Herein, 16 metal-incorporated nitrogen-doped carbon materials were designed based on the density functional theory calculation, and the adsorption mechanism of pyrolysis gas components H2, CO, CO2, CH4, and C2H6 was explored. The results indicate that metal-incorporated nitrogen-doped carbon materials generally have better adsorption effects on CO and CO2 than on H2, CH4, and C2H6. Transition metal Mo- and alkaline earth metal Mg- and Ca-incorporated nitrogen-doped carbon materials show the potential to separate CO and CO2. The mixed adsorption results of CO2 and CO further indicate that when the CO2 ratio is significantly higher than that of CO, the saturated adsorption of CO2 will precede that of CO. Overall, the three metal-incorporated nitrogen-doped carbon materials can selectively separate CO2, and the alkaline earth metal Mg-incorporated nitrogen-doped carbon material has the best performance. This study provides theoretical guidance for the design of carbon capture materials and lays the foundation for the efficient utilization of biomass pyrolysis gas.

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Triboelectric nanogenerators: the beginning of blue dream
Wanli Wang, Dongfang Yang, Xiaoran Yan, Licheng Wang, Han Hu, Kai Wang
Frontiers of Chemical Science and Engineering    2023, 17 (6): 635-678.   https://doi.org/10.1007/s11705-022-2271-y
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Wave energy is inexhaustible renewable energy. Making full use of the huge ocean wave energy resources is the dream of mankind for hundreds of years. Nowadays, the utilization of water wave energy is mainly absorbed and transformed by electromagnetic generators (EMGs) in the form of mechanical energy. However, waves usually have low frequency and uncertainty, which means low power generation efficiency for EMGs. Fortunately, in this slow current and random direction wave case, the triboelectric nanogenerator (TENG) has a relatively stable output power, which is suitable for collecting blue energy. This article summarizes the main research results of TENG in harvesting blue energy. Firstly, based on Maxwell’s displacement current, the basic principle of the nanogenerator is expounded. Then, four working modes and three applications of TENG are introduced, especially the application of TENG in blue energy. TENG currently used in blue energy harvesting is divided into four categories and discussed in detail. After TENG harvests water wave energy, it is meaningless if it cannot be used. Therefore, the modular storage of TENG energy is discussed. The output power of a single TENG unit is relatively low, which cannot meet the demand for high power. Thus, the networking strategy of large-scale TENG is further introduced. TENG’s energy comes from water waves, and each TENG’s output has great randomness, which is very unfavorable for the energy storage after large-scale TENG integration. On this basis, this paper discusses the power management methods of TENG. In addition, in order to further prove its economic and environmental advantages, the economic benefits of TENG are also evaluated. Finally, the development potential of TENG in the field of blue energy and some problems that need to be solved urgently are briefly summarized.

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Regulation of radicals by hydrogen-donor solvent in direct coal liquefaction
Wang Li, Wen-Ying Li, Xing-Bao Wang, Jie Feng
Frontiers of Chemical Science and Engineering    2022, 16 (12): 1689-1699.   https://doi.org/10.1007/s11705-022-2186-7
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Radicals are important intermediates in direct coal liquefaction. Certain radicals can cause the cleavage of chemical bonds. At high temperatures, radical fragments can be produced by the splitting of large organic molecules, which can break strong chemical bonds through the induction pyrolysis of radicals. The reaction between the formation and annihilation of coal radical fragments and the effect of hydrogen-donor solvents on the radical fragments are discussed in lignite hydrogenolysis. Using the hydroxyl and ether bonds as indicators, the effects of different radicals on the cleavage of chemical bond were investigated employing density functional theory calculations and lignite hydrogenolysis experiments. Results showed that the adjustment of the coal radical fragments could be made by the addition of hydrogen-donor solvents. Results showed that the transition from coal radical fragment to H radical leads to the variation of product distribution. The synergistic mechanism of hydrogen supply and hydrogenolysis of hydrogen-donor solvent was proposed.

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Fluorescent probes and functional materials for biomedical applications
Xi-Le Hu, Hui-Qi Gan, Fan-De Meng, Hai-Hao Han, De-Tai Shi, Shu Zhang, Lei Zou, Xiao-Peng He, Tony D. James
Frontiers of Chemical Science and Engineering    2022, 16 (10): 1425-1437.   https://doi.org/10.1007/s11705-022-2163-1
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Due to their simplicity in preparation, sensitivity and selectivity, fluorescent probes have become the analytical tool of choice in a wide range of research and industrial fields, facilitating the rapid detection of chemical substances of interest as well as the study of important physiological and pathological processes at the cellular level. In addition, many long-wavelength fluorescent probes developed have also proven applicable for in vivo biomedical applications including fluorescence-guided disease diagnosis and theranostics (e.g., fluorogenic prodrugs). Impressive progresses have been made in the development of sensing agents and materials for the detection of ions, organic small molecules, and biomacromolecules including enzymes, DNAs/RNAs, lipids, and carbohydrates that play crucial roles in biological and disease-relevant events. Here, we highlight examples of fluorescent probes and functional materials for biological applications selected from the special issues “Fluorescent Probes” and “Molecular Sensors and Logic Gates” recently published in this journal, offering insights into the future development of powerful fluorescence-based chemical tools for basic biological studies and clinical translation.

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Carbon capture for decarbonisation of energy-intensive industries: a comparative review of techno-economic feasibility of solid looping cycles
Mónica P. S. Santos, Dawid P. Hanak
Frontiers of Chemical Science and Engineering    2022, 16 (9): 1291-1317.   https://doi.org/10.1007/s11705-022-2151-5
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Carbon capture and storage will play a crucial role in industrial decarbonisation. However, the current literature presents a large variability in the techno-economic feasibility of CO2 capture technologies. Consequently, reliable pathways for carbon capture deployment in energy-intensive industries are still missing. This work provides a comprehensive review of the state-of-the-art CO2 capture technologies for decarbonisation of the iron and steel, cement, petroleum refining, and pulp and paper industries. Amine scrubbing was shown to be the least feasible option, resulting in the average avoided CO2 cost of between 62.7 €·t CO2 1 for the pulp and paper and 104.6 €·t CO21 for the iron and steel industry. Its average equivalent energy requirement varied between 2.7 (iron and steel) and 5.1 MJthkgCO2 1 (cement). Retrofits of emerging calcium looping were shown to improve the overall viability of CO2 capture for industrial decarbonisation. Calcium looping was shown to result in the average avoided CO2 cost of between 32.7 (iron and steel) and 42.9 €·t CO21 (cement). Its average equivalent energy requirement varied between 2.0 (iron and steel) and 3.7 MJthkg CO21 (pulp and paper). Such performance demonstrated the superiority of calcium looping for industrial decarbonisation. Further work should focus on standardising the techno-economic assessment of technologies for industrial decarbonisation.

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A review on the application of nanofluids in enhanced oil recovery
Jinjian Hou, Jinze Du, Hong Sui, Lingyu Sun
Frontiers of Chemical Science and Engineering    2022, 16 (8): 1165-1197.   https://doi.org/10.1007/s11705-021-2120-4
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Enhanced oil recovery (EOR) has been widely used to recover residual oil after the primary or secondary oil recovery processes. Compared to conventional methods, chemical EOR has demonstrated high oil recovery and low operational costs. Nanofluids have received extensive attention owing to their advantages of low cost, high oil recovery, and wide applicability. In recent years, nanofluids have been widely used in EOR processes. Moreover, several studies have focused on the role of nanofluids in the nanofluid EOR (N-EOR) process. However, the mechanisms related to N-EOR are unclear, and several of the mechanisms established are chaotic and contradictory. This review was conducted by considering heavy oil molecules/particle/surface micromechanics; nanofluid-assisted EOR methods; multiscale, multiphase pore/core displacement experiments; and multiphase flow fluid-solid coupling simulations. Nanofluids can alter the wettability of minerals (particle/surface micromechanics), oil/water interfacial tension (heavy oil molecules/water micromechanics), and structural disjoining pressure (heavy oil molecules/particle/surface micromechanics). They can also cause viscosity reduction (micromechanics of heavy oil molecules). Nanofoam technology, nanoemulsion technology, and injected fluids were used during the EOR process. The mechanism of N-EOR is based on the nanoparticle adsorption effect. Nanoparticles can be adsorbed on mineral surfaces and alter the wettability of minerals from oil-wet to water-wet conditions. Nanoparticles can also be adsorbed on the oil/water surface, which alters the oil/water interfacial tension, resulting in the formation of emulsions. Asphaltenes are also adsorbed on the surface of nanoparticles, which reduces the asphaltene content in heavy oil, resulting in a decrease in the viscosity of oil, which helps in oil recovery. In previous studies, most researchers only focused on the results, and the nanoparticle adsorption properties have been ignored. This review presents the relationship between the adsorption properties of nanoparticles and the N-EOR mechanisms. The nanofluid behaviour during a multiphase core displacement process is also discussed, and the corresponding simulation is analysed. Finally, potential mechanisms and future directions of N-EOR are proposed. The findings of this study can further the understanding of N-EOR mechanisms from the perspective of heavy oil molecules/particle/surface micromechanics, as well as clarify the role of nanofluids in multiphase core displacement experiments and simulations. This review also presents limitations and bottlenecks, guiding researchers to develop methods to synthesise novel nanoparticles and conduct further research.

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Catalysis of semihydrogenation of acetylene to ethylene: current trends, challenges, and outlook
Toyin D. Shittu, Olumide B. Ayodele
Frontiers of Chemical Science and Engineering    2022, 16 (7): 1031-1059.   https://doi.org/10.1007/s11705-021-2113-3
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Ethylene is an important feedstock for various industrial processes, particularly in the polymer industry. Unfortunately, during naphtha cracking to produce ethylene, there are instances of acetylene presence in the product stream, which poisons the Ziegler–Natta polymerization catalysts. Thus, appropriate process modification, optimization, and in particular, catalyst design are essential to ensure the production of highly pure ethylene that is suitable as a feedstock in polymerization reactions. Accordingly, carefully selected process parameters and the application of various catalyst systems have been optimized for this purpose. This review provides a holistic view of the recent reports on the selective hydrogenation of acetylene. Previously published reviews were limited to Pd catalysts. However, effective new metal and non-metal catalysts have been explored for selective acetylene hydrogenation. Updates on this recent progress and more comprehensive computational studies that are now available for the reaction are described herein. In addition to the favored Pd catalysts, other catalyst systems including mono, bimetallic, trimetallic, and ionic catalysts are presented. The specific role(s) that each process parameter plays to achieve high acetylene conversion and ethylene selectivity is discussed. Attempts have been made to elucidate the possible catalyst deactivation mechanisms involved in the reaction. Extensive reports suggest that acetylene adsorption occurs through an active single-site mechanism rather than via dual active sites. An increase in the reaction temperature affords high acetylene conversion and ethylene selectivity to obtain reactant streams free of ethylene. Conflicting findings to this trend have reported the presence of ethylene in the feed stream. This review will serve as a useful resource of condensed information for researchers in the field of acetylene-selective hydrogenation.

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Special issue on “Membranes and Water Treatment”
Congjie Gao, Nanping Xu, Weihong Xing
Frontiers of Chemical Science and Engineering    2022, 16 (5): 561-563.   https://doi.org/10.1007/s11705-021-2136-9
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Carbon-coated Ni-Co alloy catalysts: preparation and performance for in-situ aqueous phase hydrodeoxygenation of methyl palmitate to hydrocarbons using methanol as the hydrogen donor
Yinteng Shi, Lin Ai, Haonan Shi, Xiaoyu Gu, Yujun Han, Jixiang Chen
Frontiers of Chemical Science and Engineering    2022, 16 (4): 443-460.   https://doi.org/10.1007/s11705-021-2079-1
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Carbon-coated Ni, Co and Ni-Co alloy catalysts were prepared by the carbonization of the metal doped resorcinol-formaldehyde resins synthesized by the one-pot extended Stöber method. It was found that the introduction of Co remarkably reduced the carbon microsphere size. The metallic Ni, Co, and Ni-Co alloy particles (mainly 10–12 nm) were uniformly distributed in carbon microspheres. A charge transfer from Ni to Co appeared in the Ni-Co alloy. Compared with those of metallic Ni and Co, the d-band center of the Ni-Co alloy shifted away from and toward the Fermi level, respectively. In the in-situ aqueous phase hydrodeoxygenation of methyl palmitate with methanol as the hydrogen donor at 330 °C, the decarbonylation/decarboxylation pathway dominated on all catalysts. The Ni-Co@C catalysts gave higher activity than the Ni@C and Co@C catalysts, and the yields of n-pentadecane and n-C6n-C16 reached 71.6% and 92.6%, respectively. The excellent performance of Ni-Co@C is attributed to the electronic interactions between Ni and Co and the small carbon microspheres. Due to the confinement effect of carbon, the metal particles showed high resistance to sintering under harsh hydrothermal conditions. Catalyst deactivation is due to the carbonaceous deposition, and the regeneration with CO2 recovered the catalyst reactivity.

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