MoS presents a promising low-cost catalyst for the hydrogen evolution reaction (HER), but the understanding about its active sites has remained limited. Here we present an unambiguous study of the catalytic activities of all possible reaction sites of MoS, including edge sites, sulfur vacancies, and grain boundaries. We demonstrate that, in addition to the well-known catalytically active edge sites, sulfur vacancies provide another major active site for the HER, while the catalytic activity of grain boundaries is much weaker. The intrinsic turnover frequencies (Tafel slopes) of the edge sites, sulfur vacancies, and grain boundaries are estimated to be 7.5 s (65-75 mV/dec), 3.2 s (65-85 mV/dec), and 0.1 s (120-160 mV/dec), respectively. We also demonstrate that the catalytic activity of sulfur vacancies strongly depends on the density of the vacancies and the local crystalline structure in proximity to the vacancies. Unlike edge sites, whose catalytic activity linearly depends on the length, sulfur vacancies show optimal catalytic activities when the vacancy density is in the range of 7-10%, and the number of sulfur vacancies in high crystalline quality MoS is higher than that in low crystalline quality MoS, which may be related with the proximity of different local crystalline structures to the vacancies.

Photocatalysis has not found widespread industrial adoption, in spite of decades of active research, because the challenges associated with catalyst illumination and turnover outweigh the touted advantages of replacing heat with light. A demonstration that light can control product selectivity in complex chemical reactions could prove to be transformative. Here, we show how the recently demonstrated plasmonic behaviour of rhodium nanoparticles profoundly improves their already excellent catalytic properties by simultaneously reducing the activation energy and selectively producing a desired but kinetically unfavourable product for the important carbon dioxide hydrogenation reaction. Methane is almost exclusively produced when rhodium nanoparticles are mildly illuminated as hot electrons are injected into the anti-bonding orbital of a critical intermediate, while carbon monoxide and methane are equally produced without illumination. The reduced activation energy and super-linear dependence on light intensity cause the unheated photocatalytic methane production rate to exceed the thermocatalytic rate at 350°C.

In plasmon-enhanced heterogeneous catalysis, illumination accelerates reaction rates by generating hot carriers and hot surfaces in the constituent nanostructured metals. In order to understand how photogenerated carriers enhance the nonthermal reaction rate, the effects of photothermal heating and thermal gradients in the catalyst bed must be confidently and quantitatively characterized. This is a challenging task considering the conflating effects of light absorption, heat transport, and reaction energetics. Here, we introduce a methodology to distinguish the thermal and nonthermal contributions from plasmon-enhanced catalysts, demonstrated by illuminated rhodium nanoparticles on oxide supports to catalyze the CO methanation reaction. By simultaneously measuring the total reaction rate and the temperature gradient of the catalyst bed, the effective thermal reaction rate may be extracted. The residual nonthermal rate of the plasmon-enhanced reaction is found to grow with a superlinear dependence on illumination intensity, and its apparent quantum efficiency reaches ∼46% on a Rh/TiO catalyst at a surface temperature of 350 °C. Heat and light are shown to work synergistically in these reactions: the higher the temperature, the higher the overall nonthermal efficiency in plasmon-enhanced catalysis.

The band gap of few‐layered 2D material is one of the significant issues for the application of practical devices. Due to the outstanding electrical transport property and excellent photoresponse, 2D InSe has recently attracted rising attention. Herein, few‐layered InSe nanosheets with direct band gap are delivered by a facile liquid‐phase exfoliation approach. We have synthesized a photoelectrochemical (PEC)‐type few‐layered InSe photodetector that exhibits high photocurrent density, responsivity, and stable cycling ability in KOH solution under the irradiation of sunlight. The detective ability of such PEC InSe photodetector can be conveniently tuned by varying the concentration of KOH and applied potential suggesting that the present device can be a fitting candidate as an excellent photodetector. Moreover, extendable optimization of the photodetection performance on InSe nanosheets would further enhance the potential of the prepared InSe in other PEC‐type devices such as dye‐sensitized solar cells, water splitting systems, and solar tracking equipment.

In this work, a method is given to compute the switching angles in a multilevel converter to produce the required fundamental voltage while at the same time cancel out specified higher order harmonics. Specifically, a complete analysis is given for a seven-level converter (three dc sources), where it is shown that for a range of the modulation index , the switching angles can be chosen to produce the desired fundamental 1 = (4 dc) while making the fifth and seventh harmonics identically zero.