Latest ArticlesIn the face of multiple challenges brought by the changes of global climate and environment, developing clean energy and updating green energy storage equipment are important ways to achieve carbon peak and carbon neutrality. Aqueous batteries have become a research hotspot due to their advantages of using the multivalent charge carrier, high ionic conductivity, environmental friendliness and cost effectiveness. In this work, the Cu2Se@C (Cu2Se coated on carbon clothes) thin film with a three-dimensional braided structure is fabricated by a simple electrochemical deposition method for Cu2+ storage for the first time. Compared with the commercial Cu2Se powder, the well-designed Cu2Se@C film shows enhanced specific capacity (640 mAh/g at 0.5 A/g) and rate performance (542 mAh/g at 5 A/g) as well as superior cycling stability (82.7% capacity retention after 1000 cycles at 1 A/g). The Cu2+ storage mechanism of the Cu2Se@C electrode is based on a reversible phase transition process of Cu2Se ↔ Cu2-xSe ↔ CuSe ↔ CuSe2. In kinetic characteristic analysis, the Cu2Se@C electrode demonstrates faster Cu2+ diffusion in discharge process than charge process resulting from the phase transition and the variation of interplanar spacing. This work highlights a facile one-piece design strategy and opens a new gateway for the exploration of advanced aqueous energy storage systems.
An efficient synthesis of the electrophilic reagent, S-(1,3-dioxoisoindolin-2-yl)O,O-diethyl phosphorothioate (SDDP) is described. Moreover, the synthetic applications of SDDP wherein the transfer of the SP(O)(OEt)2 moiety occurs were investigated. In this manner, SDDP underwent facile SP(O)(OEt)2 transfer with electron-rich substrates such as ketones, indoles, and thiols to form α-phosphorothiolated ketones, 3-phosphorothiolated indoles and S-phosphorothiolated thioethers, respectively.
Integrated CO2 capture and conversion of (ICCC) is one of the most effective solutions to reduce anthropogenic CO2 emissions, which has attracted extensive public attention. Dual functional materials (DFMs), including adsorbent and catalyst, are the key components to achieve ICCC. Magnesium oxide (MgO) is an ideal adsorbent for ICCC, since it is characterized by high theoretical adsorption capacity, low cost, low energy consumption and extensive sources. It can also be used as DFMs in combination with the Ni catalysts. MgO not only can act as an adsorbent in DFMs but also enhance the catalytic performance of Ni. This review summarizes the advantages and modification methods of MgO as adsorbent and the influence of its adsorption conditions on the adsorption performance. Moreover, the important role of MgO in facilitating the catalytic conversion of CO2 is highlighted. Future research focuses are proposed for the development of MgO based DFMs with high adsorption capacity, high stability, conversion, and selectivity as well as low cost and energy consumption.
Presented here is a one-pot strategy starting from rationally designed macrocyclic precursors for the diverse construction of sophisticated ultracycles. The type and amount of the base were found to significantly influence the macrocyclization outcome. The use of 4.0 equiv. CsF resulted in ultracycles of both types A and B while the presence of CsF larger than 6.0 equiv. produced only type B ultracycles. Existence of anion template increased the total yields and affected the distribution of the ultracycles. The ultracycles can accommodate large organic dicarboxylates anions via multiple anion–π and hydrogen bonds, and show selectivity to the size-matched heptanedioate (C72−). Based on all possible species and relevant equilibrium constants as well as material and charge balances, a numerical iterative algorithm was developed and applied to fit the association constants of B2H with dicarboxylates from glutarate (C52−) to octanedioate (C82−), which gave association constants up to 103 L/mol.
Herein, we report the facile synthesis of a highly strained hexabenzocoronene-containing carbon nanoring, cyclo[4]-paraphenylene[2]-2,11-hexabenzocoronenylene ([4,2]CPHBC), as the segment of a [10,10] single-walled carbon nanotube ([10,10]SWNT). [4,2]CPHBC was synthesized based on the platinum-mediated assembly of diborylbiphenyl and diborylhexabenzocoronene, forming a tetranuclear platinum complex, followed by reductive elimination. This nanoring molecule was confirmed by NMR and HR-MS, and its photophysical properties were studied using steady-state and time-resolved spectroscopies. Moreover, the selective supramolecular host-guest interaction between [4,2]CPHBC and C60 was also investigated.
Thin-film composite (TFC) reverse osmosis (RO) membranes have attracted considerable attention in water treatment and desalination processes due to their specific separation advantages. Nevertheless, the trade-off effect between water flux and salt rejection poses huge challenges to further improvement in TFC RO membrane performance. Numerous research works have been dedicated to optimizing membrane fabrication and modification for addressing this issue. In the meantime, several reviews summarized these approaches. However, the existing reviews seldom analyzed these methods from a theoretical perspective and thus failed to offer effective optimization directions for the RO process from the root cause. In this review, we first propose a mass transfer model to facilitate a better understanding of the entire process of how water and solute permeate through RO membranes in detail, namely the migration process outside the membrane, the dissolution process on the membrane surface, and the diffusion process within the membrane. Thereafter, the water and salt mass transfer behaviors obtained from model deduction are comprehensively analyzed to provide potential guidelines for alleviating the trade-off effect between water flux and salt rejection in the RO process. Finally, inspired by the theoretical analysis and the accurate identification of existing bottlenecks, several promising strategies for both regulating RO membranes and optimizing operational conditions are proposed to further exploit the potential of RO membrane performance. This review is expected to guide the development of high-performance RO membranes from a mass transfer theory standpoint.
Borylation of 1,3-enynes with bis(boronate) compounds often ends up with the formation of hydroborylated products, leaving the diborylation of 1,3-enynes for the formation of 1,4-diborylated allenes to be challenging. Herein, a copper-catalyzed chemo-, regio-, and stereo-selective diborylation of 1,3-enynes for the efficient construction of 1,4-diborylated allenes under base-free conditions was reported. A wide range of 1,3-enynes bearing various functional groups can participant in the reaction and afforded the corresponding 1,4-diborylated allenes in good to excellent yields, which was enabled by the protocol of Bpin to BF3K conversion. the borylcopper species was supposed to selectively attack the C–C triple bond of the 1,3-enynes.
Molecular recognition in water, the biological solvent, always receives significant research focus in supramolecular chemistry. The mechanisms of molecular recognition in water is key to comprehending biological processes at the molecular level. Over the past five decades, supramolecular chemists have developed a vast array of synthetic receptors with highly diverse structures and recognition properties. Among them, cyclophanes represent an important family of macrocyclic receptors that have been extensively explored. The aromatic moieties in cyclophanes not only facilitate chemical modifications to impart water solubility but also enable forming hydrophobic cavities for guest inclusion in aqueous environments. Pioneered by Koga et al., who reported the first inclusion complex of cyclophanes in water and solid state, numerous water-soluble cyclophanes, including derivatives of blue box, calixarenes, resorcinarenes, pillararenes, octopusarenes, biphenarenes, coronarenes, and naphthotubes, etc., have been synthesized and subjected to investigation of the recognition capabilities in aqueous solutions. This review provides an overview of cyclophane receptors designed to bind organic guests in water. We categorize them into two classes based on the modifications made to their hydrophobic cavities: those with "exo-functionalized hydrophobic cavities" and those with "endo-functionalized hydrophobic cavities". We introduce their distinctive features and discuss strategies to enhance recognition affinity and selectivity. This review aims to inspire the development of novel synthetic receptors with intriguing properties and foster practical applications of cyclophanes.
Chiral alcohols and amines are important structural units widely existing in pharmaceuticals, agrochemicals, and food additives. Dynamic kinetic resolution (DKR) is an efficient strategy to deliver optically active alcohols and amines from their racemates. For the development of DKR method, racemization catalyst plays as a crucial element with the requirement of compatibility with the kinetic resolution (KR) system. In this paper, recent advance in the catalytic racemization of secondary alcohols and amines is summarized based on different types of racemizing intermediates, which are redox racemization via ketone/imine intermediates, racemization via radical intermediates, and racemization via carbocation intermediates. Enzymatic racemization of secondary alcohols and amines is also enclosed.
The dynamic RNA modifications have been viewed as new posttranscriptional regulator in modulating gene expression as well as in a broad range of physiological processes. N1-methyladenosine (m1A) is one of the most prevalent modifications existing in multiple types of RNAs. In-depth investigation of the functions of m1A requires the site-specific assessment of m1A stoichiometry in RNA. Herein, we established a demethylase-assisted method (DA-m1A) for the site-specific detection and quantification of m1A in RNA. N1-methyl group in m1A could result in the stalling of reverse transcription at m1A site, thus producing the truncated cDNA. E. coli AlkB is a demethylase that can demethylate m1A to produce adenine in RNA, thus generating full-length cDNA from AlkB-treated RNA. Evaluation of the produced amounts of full-length cDNA by quantitative real-time PCR can achieve the site-specific detection and quantification of m1A in RNA. With the DA-m1A method, we examined and successfully confirmed the previously well-characterized m1A sites in various types of RNAs with low false positive rate. In addition, we found that the level of m1A was significantly decreased at the bromodomain containing 2 (BRD2) mRNA position 1674 and CST telomere replication complex component 1 (CTC1) mRNA position 5643 in human hepatocellular carcinoma tissues. The results suggest that these two m1A sites in mRNA may be involved in liver tumorigenesis. Taken together, the DA-m1A method is simple and enables the rapid, cost-effective, and site-specific detection and quantification of m1A in RNA, which provides a valuable tool to decipher the functions of m1A in human diseases.
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