Bulk amorphous materials have been studied extensively and are used widely. Yet, their atomic arrangement remains an open issue. They are generally believed to be Zachariasen continuous random networks (Z-CRNs) 1 , but recent experimental evidence favours the competing crystallite model in the case of amorphous silicon 2-4 .Corresponding questions in 2D materials are wide open. Here we report the synthesis of centimetre-scale, freestanding, continuous, and stable monolayer amorphous carbon (MAC), topologically distinct from disordered graphene, by laser-assisted chemical vapour deposition 5 . Unlike bulk materials, the amorphous structure of MAC can be determined by atomic-resolution imaging. Extensive characterisation reveals complete absence of long-range periodicity and a threefold-coordinated structure with a wide distribution of bond lengths, bond angles, and 5-, 6-, 7-, and 8-member rings. The ring distribution is not a Z-CRN but resembles the competing (nano)crystallite model 6 . A corresponding model has been constructed and enables density-functional-theory calculations of MAC properties, in accord with observations. Direct measurements

Rational design of highly efficient bifunctional electrocatalysts based on 3D transition-metal-based materials for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is of great importance for sustainable energy conversion processes. Herein, a novel strategy involving outer and inner structural engineering is developed for superior water splitting via in situ vertical growth of 2D amorphous FePO nanosheets on Ni foam (Am FePO /NF). Careful experiments and density functional theory calculations show that the inner and outer structural engineering contributing to the synergistic effects of 2D morphology, amorphous structure, conductive substrate, and Ni-Fe mixed phosphate lead to superior electrocatalytic activity toward OER and HER. Furthermore, a two-electrode electrolyzer assembled using Am FePO /NF as an electrocatalyst at both electrodes gives current densities of 10 and 100 mA cm at potentials of 1.54 and 1.72 V, respectively, which is comparable to the best bifunctional electrocatalyst reported in the literature. The strategies, introduced in the present work, may open new opportunities for the rational design of other 3D transition-metal-based electrocatalyst through an outer and inner structural control to strengthen the electrocatalytic performance.

We present a one-pot colloidal route to synthesize VSe2, a new type of metallic single-layer nanosheet. The ∼0.4 nm thick VSe2 single-layer nanosheets possess extraordinary electrocatalytic hydrogen evolution reaction (HER) performance with a low onset overpotential of 108 mV, a small Tafel slope of 88 mV per decade, and an exceptional overpotential of 206 mV at a current density of 10 mA cm(-2).

Large scale implementation of electrochemical water splitting for hydrogen evolution requires cheap and efficient catalysts to replace expensive platinum. Molybdenum disulfide is one of the most promising alternative catalysts but its intrinsic activity is still inferior to platinum. There is therefore a need to explore new active site origins in molybdenum disulfide with ultrafast reaction kinetics and to understand their mechanisms. Here, we report a universal cold hydrogen plasma reduction method for synthesizing different single atoms sitting on two-dimensional monolayers. In case of molybdenum disulfide, we design and identify a new type of active site, i.e., unsaturated Mo single atoms on cogenetic monolayer molybdenum disulfide. The catalyst shows exceptional intrinsic activity with a Tafel slope of 35.1 mV dec −1 and a turnover frequency of ~10 3 s-1 at 100 mV, based on single flake microcell measurements. Theoretical studies indicate that coordinately unsaturated Mo single atoms sitting on molybdenum disulfide increase the bond strength between adsorbed hydrogen atoms and the substrates through hybridization, leading to fast hydrogen adsorption/desorption kinetics and superior hydrogen evolution activity. This work shines fresh light on preparing highly-efficient electrocatalysts for water splitting and other electrochemical processes, as well as provides a general method to synthesize single atoms on two-dimensional monolayers.

Epitaxial synthesis of monolayer PtSe2 single crystal on MoSe2 with strong interlayer coupling