With the advancement of social process, the resource problem is becoming more prominent, biomass materials come into being, and it is becoming more and more important to explore and prepare efficient and multifunctional biomass materials to alleviate the problems of energy storage and water pollution. In this paper, nitrogen-doped hierarchical porous carbon materials (NRRC) were produced by one-step carbonization of withered rose as raw material and melamine as nitrogen source with KOH-activated porosification. The resulting nitrogen-doped porous carbon material had the most abundant pores and the best microspherical graded pore structure, with a specific surface area of up to 1393 m2·g–1, a pore volume of 0.68 cm3·g–1, and a nitrogen-doped content of 5.52%. Electrochemical tests showed that the maximum specific capacitance of NRRC in the three-electrode system was 346.4 F·g–1 (0.5 A·g–1), which was combined with favorable capacitance retention performance and cycling stability. The NRRC//NRRC symmetric supercapacitors were further assembled, and the maximum energy density of a single device was 23.88 Wh·kg–1, which still maintains excellent capacitance retention and cyclic charging/discharging stability. For example, the capacitance retention rate was always close to 96.27% with almost negligible capacitance loss after 10000 consecutive charge/discharge cycles (current density: 10 A·g–1). Regardless of the three-electrode or two-electrode system, the super capacitive performance of NRRC porous carbon materials was comparable to the electrochemical performance of many reported biomass porous carbon materials, which showed better energy storage advantages and practical application potential. In addition, NRRC porous carbon materials had excellent water purification ability. The dye adsorption test confirmed that NRRC had a high adsorption capacity (491.47 mg·g–1) for methylene blue. This undoubtedly also showed a potential and promising avenue for high value-added utilization of this material.
Carbon dioxide fixation presents a potential solution for mitigating the greenhouse gas issue. During carbon dioxide fixation, C1 compound reduction requires a high energy supply. Thermodynamic calculations suggest that the energy source for cofactor regeneration plays a vital role in the effective enzymatic C1 reduction. Hydrogenase utilizes renewable hydrogen to achieve the regeneration and supply cofactor nicotinamide adenine dinucleotide (NADH), providing a driving force for the reduction reaction to reduce the thermodynamic barrier of the reaction cascade, and making the forward reduction pathway thermodynamically feasible. Based on the regeneration of cofactor NADH by hydrogenase, and coupled with formaldehyde dehydrogenase and formolase, a favorable thermodynamic mode of the C1 reduction pathway for reducing formate to dihydroxyacetone (DHA) was designed and constructed. This resulted in accumulation of 373.19 μmol·L–1 DHA after 2 h, and conversion reaching 7.47%. These results indicate that enzymatic utilization of hydrogen as the electron donor to regenerate NADH is of great significance to the sustainable and green development of bio-manufacturing because of its high economic efficiency, no by-products, and environment-friendly operation. Moreover, formolase efficiently and selectively fixed the intermediate formaldehyde (FALD) to DHA, thermodynamically pulled formate to efficiently reduce to DHA, and finally stored the low-grade renewable energy into chemical energy with high energy density.
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.
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.
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.
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.
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.
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
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.
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.