Atmospheric carbon dioxide (CO2) is assimilated by the most abundant but sluggish enzyme, ribulose-1,5-bisphosphate carboxylase/oxygenase (Rubisco). Here we show that acetylation of lysine residues of the Rubisco large subunit (RbcL), including Lys201 and Lys334 in the active sites, may be an important mechanism in the regulation of Rubisco activities. It is well known that Lys201 reacts with CO2 for carbamylation, a prerequisite for both carboxylase and oxygenase activities of Rubisco, and Lys334 contacts with ribulose-1,5-bisphosphate (RuBP). The acetylation level of RbcL in plants is lower during the day and higher at night, inversely correlating with the Rubisco carboxylation activity. A search of the chloroplast proteome database did not reveal a canonical acetyltransferase; instead, we found that a plant-derived metabolite, 7-acetoxy-4-methylcoumarin (AMC), can non-enzymatically acetylate both native Rubisco and synthesized RbcL peptides spanning Lys334 or Lys201. Furthermore, lysine residues were modified by synthesized 4-methylumbelliferone esters with different electro- and stereo-substitutes, resulting in varied Rubisco activities. 1-Chloroethyl 4-methylcoumarin-7-yl carbonate (ClMC) could transfer the chloroethyl carbamate group to lysine residues of RbcL and completely inactivate Rubisco, whereas bis(4-methylcoumarin-7-yl) carbonate (BMC) improved Rubisco activity through increasing the level of Lys201 carbamylation. Our findings indicate that RbcL acetylation negatively regulates Rubisco activity, and metabolic derivatives can be designed to dissect and improve CO2 fixation efficiency of plants through lysine modification.
The search for new inorganic electrides has attracted significant attention due to their potential applications in transparent conductors, battery electrodes, electron emitters, as well as catalysts for chemical synthesis. However, only a few inorganic electrides have been successfully synthesized thus far, limiting the variety of electride examples. Here, we show the stabilization of inorganic electrides in the Ti-rich Ti-O system through first-principles calculations in conjunction with swarm-intelligence-based CALYPSO method for structure prediction. Besides the known Ti-rich stoichiometries of Ti 2 O, Ti 3 O, and Ti 6 O, two hitherto unknown Ti 4 O and Ti 5 O stoichiometries are predicted to be thermodynamically stable at certain pressure conditions. We found that these Tirich Ti-O compounds are primarily zero-dimensional electrides with excess electrons confined in the atom-sized lattice voids or between the cationic layers playing the role as anions. The underlying mechanism behind the stabilization of electrides has been rationalized in terms of the excess electrons provided by Ti atoms and their accommodation of excess electrons by multiple cavities and layered atomic packings. The present results provide a viable direction for searching for practical electrides in the technically important Ti-O system.
In this study, we introduced an ordered metal–semiconductor–molecular system and investigated the surface-enhanced Raman scattering (SERS) effect. The carrier distribution and density can be easily monitored by changing the thickness of the Cu2S film on the surface of the Ag monolayer under different laser excitations. Meanwhile, different laser wavelengths were selected for investigating the enhancement mechanism of the system based on the viewpoint of the number of carriers and changes in the excitation energy. During this process, we found that the SERS peaks located at 1586 cm–1 changed significantly because the intensity can be “borrowed” from exited transition and the molecule-to-semiconductor transition. In combination with the theories of Albrecht and Lombardi, this phenomenon was analyzed in detail, and the experimental results and theoretical research match well. This research regarding the semiconductor-based SERS substrates will expand the basic theory of SERS enhancement and provide a theoretical basis for optical and biological applications.
A novel 2D porous NiCoSe nanosheet arrays were grown on Ni foam using ZIF-67 as precursors, which exhibited outstanding bifunctional electrocatalytic activity and superior durability for overall water splitting.
We discuss how the controllable carrier influences the localized surface plasmon resonance (LSPR) and charge transfer (CT) in the same system based on ultraviolet-visible and surface-enhanced Raman scattering (SERS) measurements. The LSPR can be easily tuned from 580 to 743 nm by changing the sputtering power of CuS in the Ag and CuS composite substrate. During this process, surprisingly, we find that the LSPR is proportional to the sputtering power of CuS. This observation indicates that LSPR can be accurately adjusted by changing the content of the semiconductor, or even the carrier density. Moreover, we characterize the carrier density through the detection of the Hall effect to analyze the Raman shift caused by CT and obtain the relationships between them. These fundamental discussions provide a guideline for tunable LSPR and the investigation of CT.
SUMMARYMost of the recent studies about the photovoltaic cell-thermoelectric generator (PV-TEG) hybrid system pay their attention to silicon PV cells. This paper is to estimate the feasibility and features of the integrated system consisting of the emerging perovskite solar cells and thermoelectric modules. The results in this paper show that the temperature coefficient of the perovskite solar cell is lower than 2‰. Because of such a lower temperature coefficient, the efficiency of the perovskite solar cell-TEG hybrid system can amount to 18.6%, while the efficiency of the single perovskite solar cell is 17.8%. Therefore, the perovskite solar cell is a reasonable choice for the PV-TEG hybrid system. By altering the thermal concentration, the volume of the TEG material can be decreased, and the cost of the hybrid system can be remarkably reduced. To study the influence of the thermal concentration on the performance of the hybrid system, a three-dimensional numerical model of the hybrid system is developed in this paper. When the thermal concentration ration is lower than 100, the temperature drop is lower than 3 K, and the decline in the conversion efficiency caused by the thermal concentration can be neglected for the proposed PV-TEG hybrid system.
Hexagonal close-packed tilted Ag nanorod arrays that exhibit excellent uniformity and reproducibility were prepared. The tilt angle was easily controlled by regulating the sputtering angle, accompanied by a reduction and constancy in the gap size of adjacent nanorods, which is 30° and 90° relative to the sputtering direction. The surface enhanced Raman spectroscopy (SERS) technique was used to characterize the interaction of tilted Ag nanorod arrays with polarized laser excitation. Interestingly, the SERS polarization-dependence increased with increasing tilt angle of the Ag nanorods. To elucidate the essential factors responsible for this SERS result, three-dimensional (3D) electromagnetic enhancement distribution for the proposed system was numerically simulated based on p- and s-polarization excitation. Most importantly, the fundamental reasons for the polarization dependence of SERS were obtained by a quantitative 3D numerical simulation of hotspot distribution for adjacent nanorods.
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