Hong Pang

Targeted Synthesis of 2H- and 1T-Phase MoS2 Monolayers for Catalytic Hydrogen Evolution.

Through a facile and effective strategy by employing lithium molten salts the controlled synthesis of 2H- and 1T-MoS2 monolayers with high-yield production is achieved. Both phases of MoS2 monolayers exhibit high stabilities. When used as a catalyst for hydrogen evolution, these phased MoS2 monolayers deliver respective advantages in the field of electro- and photo-catalytic hydrogen evolution.

Engineering the crystallinity of MoS2 monolayers for highly efficient solar hydrogen production

As a promising non-precious catalyst for the hydrogen evolution reaction (HER), molybdenum disulfide (MoS2), which is known to contain highly active edge sites and an inert basal plane, has attracted extensive interest. More recently, its amorphous counterpart has been found to have a higher HER activity, making it important to explore the effect of crystallinity on the HER performance of monolayer MoS2. However, the posed technological challenges of preparing crystallinity tunable 2H–MoS2 monolayers hinder their further study. In this work, we report the successful synthesis of crystallinity-dependent MoS2 monolayers through liquid exfoliation of the corresponding crystallinity-controllable bulk precursors. Excellent cocatalytic performances of the proposed MoS2 monolayers for the photocatalytic HER were achieved and determined by their crystallinity. An apparent quantum efficiency as high as 71.6% can be achieved for the lowest crystalline monolayer MoS2 over cadmium sulfide under visible light irradiation at 420 nm. This work provides a facile way to synthesise crystallinity controllable MoS2 monolayers and elucidates that the HER activity can be further enhanced through crystallinity engineering, providing a new strategy to enhance the HER activity of monolayer MoS2.

Improved Photocatalytic H2 Evolution over G‐Carbon Nitride with Enhanced In‐Plane Ordering

A series of rod-like porous graphitic-carbon nitrides (short as CNs) with enhanced in-plane ordering have been fabricated through self-assembled heptazine hydrate precursors for the first time. By controlling the calcination of the preformed precursors with different temperature-rising rates, the resulted CNs (SAHEP-CNs-1) with the most ordered and least stacked graphitic planar are showing a tremendously improved hydrogen evolution rate of 420 μmol h-1 under visible light and a remarkable apparent quantum efficiency of 8.9% at 420 nm, which is among the highest values for C3 N4 -related photocatalysts in the literature. This work discloses that enhancing in-plane ordering is one critical factor for improving the photocatalytic H2 evolution of carbon nitride, which is an effective solution to prolong the lifetime of charge carriers by accelerating the charge transport and separation within the graphitic planar. This finding would present a facial strategy for the designing of efficient organic semiconductors for photocatalysis.

Elemental Boron for Efficient Carbon Dioxide Reduction under Light Irradiation

The photoreduction of CO2 is attractive for the production of renewable fuels and the mitigation of global warming. Herein, we report an efficient method for CO2 reduction over elemental boron catalysts in the presence of only water and light irradiation through a photothermocatalytic process. Owing to its high solar-light absorption and effective photothermal conversion, the illuminated boron catalyst experiences remarkable self-heating. This process favors CO2 activation and also induces localized boron hydrolysis to in situ produce H2 as an active proton source and electron donor for CO2 reduction as well as boron oxides as promoters of CO2 adsorption. These synergistic effects, in combination with the unique catalytic properties of boron, are proposed to account for the efficiency of the CO2 reduction. This study highlights the promise of photothermocatalytic strategies for CO2 conversion and also opens new avenues towards the development of related solar-energy utilization schemes.

Semiconductor-Based Photoelectrochemical Conversion of Carbon Dioxide: Stepping Towards Artificial Photosynthesis

The photoelectrochemical (PEC) carbon dioxide reduction process stands out as a promising avenue for the conversion of solar energy into chemical feedstocks, among various methods available for carbon dioxide mitigation. Semiconductors derived from cheap and abundant elements are interesting candidates for catalysis. Whether employed as intrinsic semiconductors or hybridized with metallic cocatalysts, biocatalysts, and metal molecular complexes, semiconductor photocathodes exhibit good performance and low overpotential during carbon dioxide reduction. Apart from focusing on carbon dioxide reduction materials and chemistry, PEC cells towards standalone devices that use photohybrid electrodes or solar cells have also been a hot topic in recent research. An overview of the state-of-the-art progress in PEC carbon dioxide reduction is presented and a deep understanding of the catalysts of carbon dioxide reduction is also given.

Interfacing Photosynthetic Membrane Protein with Mesoporous WO3 Photoelectrode for Solar Water Oxidation

Photosynthetic biocatalysts are emerging as a new class of materials, with their sophisticated and intricate structure, which promise improved remarkable quantum efficiency compared to conventional inorganic materials in artificial photosynthesis. To break the limitation of efficiency, the construction of bioconjugated photo-electrochemical conversion devices has garnered substantial interest and stood at the frontier of the multidisciplinary research between biology and chemistry. Herein, a biohybrid photoanode of a photosynthetic membrane protein (Photosystem II (PS II)), extracted from fresh spinach entrapped on mesoporous WO3 film, is fabricated on fluorine-doped tin oxide. The PS II membrane proteins are observed to communicate with the WO3 electrode in the absence of any soluble redox mediators and sacrificial reagents under the visible light of the solar spectrum, even to 700 nm. The biohybrid electrode undergoes electron transfer and generates a significantly enhanced photocurrent compared to previously reported PS II-based photoanodes with carbon nanostructures or other semiconductor substrates for solar water oxidation. The maximum incident photon-to-current conversion efficiency reaches 15.24% at 400 nm in the visible light region. This work provides some insights and possibilities into the efficient assembly of a future solar energy conversion system based on visible-light-responsive semiconductors and photosynthetic proteins.