Hydrogen spillover (HSo) has emerged to upgrade the hydrogen evolution reaction (HER) activity of Pt‐support electrocatalysts, but it is not applicable to the deprotonated oxygen evolution reaction (OER). Non‐precious catalysts that can perform well in both HSo and deprotonation (DeP) are extremely desirable for a sustainable hydrogen economy. Herein, an affordable MoS2/NiPS3 vertical heterostructure catalyst is presented to synergize HSo and DeP for efficient water electrolysis. The internal polarization field (IPF) is clarified as the driving force of HSo in HER electrocatalysis. The HSo from the MoS2 edge to NiPS3 can activate the NiPS3 basal plane to boost the HER activity of the MoS2/NiPS3 heterostructure (112 mV vs reversible hydrogen electrode (RHE) at 10 mA cm–2), while for OER, the IPF in the heterostructure can facilitate the hydroxyl diffusion and render MoS2‐to‐NiPS3/P‐to‐S dual‐pathways for DeP. As a result, the stacking of OER‐inactive MoS2 on the NiPS3 surface still brings intriguing OER enhancements. With them serving as electrode couples, the overall water splitting is attested stably with a cell voltage of 1.64 V at 10 mA cm−2. This research puts forward the IPF as the criterion in the rational design of HSo/DeP‐unified non‐precious catalysts for efficient water electrolysis.

A monolayer α-Fe2O3 inverse opal film with single-crystalline rotocenters shows reversible NO2 p–n sensing switches tuned by a T–C transition diagram.

Electrocatalytic splitting of water holds the fossil-free premise for H 2 production, which couples cathodic hydrogen and anodic oxygen evolution reactions (HER/OER). [1] Kinetically driving water electrolysis (WE) requires efficient and stable catalysts to reduce the overpotentials for both HER and OER. [2] During practical WE operations, the electrolyte's pH change is a critical challenge for the activity and stability retention of the electrocatalysts. [3] Therefore, there is an urgent need to develop robust electrocatalysts for wide pH conditions to ensure work efficiency and reduce usage costs. Although Pt-group metals are endowed with active and pH-robust HER/OER properties, the costliness and scarcity greatly limit their sustainable deployments in WE. [4] In this regard, rationalizing non-precious pHrobust catalysts is the top priority of current research for water splitting. Electronic level adjustment is the fundamental technique for the rational design of advanced non-precious catalysts. [5] As known, the d-band (ε d ) and p-band center (ε p ) to Fermi level can well reflect the intermediates' adsorption energies and activation energy barriers during HER/ OER catalysis. [6] Currently, the d-band center level of 3d-metal sites is widely considered to be effective descriptors for HER and OER. [5a] However, the metal sites are not the actual active catalytic centers in some systems, [6c] and the p-band center of non-metal atoms should be revisited together with ε d . Hence, the synergic tuning of d/p-band center will be the design criterion for the innovation of economic, robust, and efficient WE catalysts.Interface engineering is deemed as an effective measure to achieve the d-band center regulation in terms of the interfacial charge transfer between the components. [7] In addition, the heterostructure can exhibit the protection and lattice confinement effect on the surface active atoms, modifying the stability and electronic structure by lattice distortion. [8] Current reports on transition metal heterostructures are mainly crystalline-crystalline complexes, and the interfacial atomic distortion will be hindered by lattice resistance or structural rigidity to some extent. [9] In this context, the establishment of an amorphous-crystalline Rationalizing non-precious pH-robust electrocatalysts is a crucial priority and required for multi-scenario hydrogen production customization. Herein, an amorphous-crystalline CoBO x /NiSe heterostructure is theoretically profiled and constructed for efficient and pH-robust water electrolysis. The crystalline lattice confinement induces a CoCo bond shortening and a B-site delocalization on amorphous CoBO x , resulting in a decreased d-p band center difference (Δε d-p ) toward the balanced intermediates adsorption/desorption. Accordingly, the CoBO x /NiSe heterostructure exhibits efficient and robust hydrogen/oxygen evolution reaction (HER/OER) catalytic activity in different electrolytes. Of particular note, it achieves ultralow overpotentials in both the beyon...

Herein, we discuss the study of solvation dynamics of lithium-succinonitrile (SN) plastic crystalline electrolytes by ultrafast vibrational spectroscopy. The infrared absorption spectra indicated that the CN stretch of the Li(+) bound and unbound succinonitrile molecules in a same solution have distinct vibrational frequencies (2276 cm(-1)vs. 2253 cm(-1)). The frequency difference allowed us to measure the rotation decay times of solvent molecules bound and unbound to Li(+) ion. The Li(+) coordination number of the Li(+)-SN complex was found to be 2 in the plastic crystal phase (22 °C) and 2.5-3 in the liquid phase (80 °C), which is independent of the concentration (from 0.05 mol kg(-1) to 2 mol kg(-1)). The solvation structures along with DFT calculations of the Li(+)-SN complex have been discussed. In addition, the dissociation percentage of lithium salt was also determined. In 0.5 mol kg(-1) LiBF4-SN solutions at 80 °C, 60% ± 10% of the salt dissociates into Li(+), which is bound by 2 or 3 solvent molecules. In the 0.5 mol kg(-1) LiClO4-SN solutions at 80 °C, the salt dissociation ratio can be up to 90% ± 10%.

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Herein, this is the first report on the dissolution of cellulose at room temperature (R.T.) by using the AlCl3/ZnCl2·4H2O solvent system. Cellulose with broad degrees of polymerization (DP), even those...

The innovation of NO2 gas sensors is highly desirable in environmental monitoring and human safety. Herein, a macroporous SnO2/MoS2 inverse opal hierarchitecture has been constructed with substantial interface charge transfer,...