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Transition metal phosphides (TMPs) have emerged as an alternative to precious metals as efficient and low‐cost catalysts for water electrolysis. Elemental doping and morphology control are effective approaches to further improve the performance of TMPs. Herein, Fe‐doped CoP nanoframes (Fe‐CoP NFs) with specific open cage configuration were designed and synthesized. The unique nano‐framework structured Fe‐CoP material shows overpotentials of only 255 and 122 mV at 10 mA cm−2 for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), respectively, overwhelming most transition metal phosphides. For overall water splitting, the cell voltage is 1.65 V for Fe‐CoP NFs at a current density of 10 mA cm−2, much superior to what is observed for the classical nanocubic structures. Fe‐CoP NFs show no activity degradation up to 100 h which contrasts sharply with the rapidly decaying performance of noble metal catalyst reference. The superior electrocatalytic performance of Fe‐CoP NFs due to abundant accessible active sites, reduced kinetic energy barrier, and preferable *O‐containing intermediate adsorption is demonstrated through experimental observations and theoretical calculations. Our findings could provide a potential method for the preparation of multifunctional material with hollow structures and offer more hopeful prospects for obtaining efficient earth‐abundant catalysts for water splitting. [ABSTRACT FROM AUTHOR]

Herein, the concept of "inverted" (the mode "molecules mainly interact with cations") deep eutectic solvents (DESs) is proposed. A strategy to form inverted DESs by host‐guest interactions was developed, and thus numerous DESs could be designed and formed by a combination of host and guest molecules. These liquids are expected to be used as nonaqueous electrolytes in potassium‐ion batteries or other fields for further exploration. [ABSTRACT FROM AUTHOR]

Eutectic molecular liquids (EMLs) based on hydrogen‐bonding interaction and π–π stacking were prepared. We found that the thermodynamic properties like initial decomposition temperature and glass transition temperature of EMLs are mainly dominated by the hydrogen bond donor, which is beneficial for designing and preparing new EMLs. These new liquid systems could be applied in the field of environmental and material science. [ABSTRACT FROM AUTHOR]

Lithium-based deep eutectic solvents (DESs) are potential and promising electrolytes for energy-storing devices such as the lithium-ion battery and supercapacitor due to their greenness, low cost, favorable stability, and ease of synthesis. LiTf2N (lithium bis(trifluoromethylsulfonyl)imide):NMA (N-methylacetamide) is a liquid due to the strong intermolecular H-bonding interaction between the H-bonding acceptor (HBA, LiTf2N) and H-bonding donor (HBD, NMA). The properties (melting point, conductivity, viscosity, etc.) of LiTf2N:NMA change with the evaporation of NMA from LiTf2N:NMA, which would further influence the performance of the energy-storing devices. The evaporation of DES should be determined by the intermolecular interactions. Here, for the first time, the dynamic process of evaporation and intermolecular interactions of the DES LiTf2N:NMA at room temperature were investigated and we find that the evaporation mechanism of the DES LiTf2N:NMA can be divided into three stages. In the first stage (before 110 min), the H-bonding interaction between O in LiTf2N and NH in NMA is disrupted before destruction of the coordinating interaction related to amide II C=O and Li cation. In the second stage (from 110 min to 270 min), the change of coordinating interaction related to amide II C=O and Li cation is also higher than that of the H-bonded interaction. In the third stage (after 270 min), evaporation of NMA from LiTf2N:NMA has very little influence on the environment of LiTf2N:NMA. This work provides a guide for designing DESs as electrolytes for energy-storing devices such as the lithium-ion battery and supercapacitor. [ABSTRACT FROM AUTHOR]

We report the synthesis of nanostructured Fe3S4 from deep eutectic solvents via a one-step solvothermal method. The as-obtained Fe3S4 catalyst was capable of electrochemically reducing N2 to NH3 under ambient conditions, and exhibits a high NH3 yield (75.4 μg h−1 mg−1cat.) and faradaic efficiency (6.45%) at −0.4 V vs. a reversible hydrogen electrode. [ABSTRACT FROM AUTHOR]

Chalcogen bonding (ChB) interactions have drawn intensive attention in the last few decades as interesting alternatives to hydrogen bonding. The applications of ChB were mostly centered on the solid state and have rarely been explored in solution. In this work, a novel strategy for forming ChB-based deep eutectic solvents (DESs) was exploited. We set forth the formation, physicochemical properties, and interaction sites in detail. This work not only provides a new idea to design DES systems but also to exploit the potential application of ChB complexes.

Solar-driven nitrogen fixation remains a significant challenge. Graphitic carbon nitride (g-C 3 N 4 ) is considered as a promising visible light photocatalyst. However, the photocatalytic performance of g-C 3 N 4 is unsatisfactory because of the random transfer of charge carriers in the plane and the low activation efficiency of the reactants. Herein, amorphous ZrO 2 was used as a robust cocatalyst of g-C 3 N 4 to increase the NH 3 production activity. The g-C 3 N 4 /ZrO 2 lamellar composites were constructed by a simple one-step pyrolysis of the deep eutectic solvent ZrOCl 2 ·8H 2 O/urea. The optimum NH 4 + yield could reach as high as 1446 μmol·L -1 ·h -1 at 30 wt % ZrO 2 in the g-C 3 N 4 /ZrO 2 composites, with an apparent quantum efficiency over 2.14% at 400 nm. It is 7.9 times that of pristine g-C 3 N 4 and 27.5 times that of ZrO 2 . The introduction of amorphous ZrO 2 restrained the hydrogen generation, and the amorphous ZrO 2 and g-C 3 N 4 together contribute to the rapid photoproduced electron transfer of less electron-hole pair recombination.

Lithium-based deep eutectic solvents (DESs) are potential and promising electrolytes for energy-storing devices such as the lithium-ion battery and supercapacitor due to their greenness, low cost, favorable stability, and ease of synthesis. LiTf2N (lithium bis(trifluoromethylsulfonyl)imide):NMA (N-methylacetamide) is a liquid due to the strong intermolecular H-bonding interaction between the H-bonding acceptor (HBA, LiTf2N) and H-bonding donor (HBD, NMA). The properties (melting point, conductivity, viscosity, etc.) of LiTf2N:NMA change with the evaporation of NMA from LiTf2N:NMA, which would further influence the performance of the energy-storing devices. The evaporation of DES should be determined by the intermolecular interactions. Here, for the first time, the dynamic process of evaporation and intermolecular interactions of the DES LiTf2N:NMA at room temperature were investigated and we find that the evaporation mechanism of the DES LiTf2N:NMA can be divided into three stages. In the first stage (before 110 min), the H-bonding interaction between O in LiTf2N and NH in NMA is disrupted before destruction of the coordinating interaction related to amide II C[double bond, length as m-dash]O and Li cation. In the second stage (from 110 min to 270 min), the change of coordinating interaction related to amide II C[double bond, length as m-dash]O and Li cation is also higher than that of the H-bonded interaction. In the third stage (after 270 min), evaporation of NMA from LiTf2N:NMA has very little influence on the environment of LiTf2N:NMA. This work provides a guide for designing DESs as electrolytes for energy-storing devices such as the lithium-ion battery and supercapacitor.