Biomass has incredible potential as an alternative to fossil fuels for energy production that is sustainable for the future of humanity. Hydrogen evolution from photocatalytic biomass conversion not only produces valuable carbon-free energy in the form of molecular hydrogen but also provides an avenue of production for industrially relevant biomass products. This photocatalytic conversion can be realized with efficient, sustainable reaction materials (biomass) and inexhaustible sunlight as the only energy inputs. Reported herein is a general strategy and mechanism for photocatalytic hydrogen evolution from biomass and biomass-derived substrates (including ethanol, glycerol, formic acid, glucose, and polysaccharides). Recent advancements in the synthesis and fundamental physical/mechanistic studies of novel photocatalysts for hydrogen evolution from biomass conversion are summarized. Also summarized are recent advancements in hydrogen evolution efficiency regarding biomass and biomass-derived substrates. Special emphasis is given to methods that utilize unprocessed biomass as a substrate or synthetic photocatalyst material, as the development of such will incur greater benefits towards a sustainable route for the evolution of hydrogen and production of chemical feedstocks.

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Introducing amorphous and ultrathin nanosheets of transition bimetal phosphate arrays that are highly active in the oxygen evolution reaction (OER) as shells over an electronically modulated crystalline core with low hydrogen absorption energy for an excellent hydrogen evolution reaction (HER) can boost the sluggish kinetics of the OER and HER in alkaline electrolytes. Therefore, in this study, ultrathin and amorphous cobalt‐nickel‐phosphate (CoNiPO x ) nanosheet arrays are deposited over vanadium (V)‐doped cobalt‐nitride (V 3% ‐Co 4 N) crystalline core nanowires to obtain amorphous‐shell@crystalline‐core mesoporous 3D‐heterostructures (CoNiPO x @V‐Co 4 N/NF) as bifunctional electrocatalysts. The optimized electrocatalyst shows extremely low HER and OER overpotentials of 53 and 270 mV at 10 mA cm −2 , respectively. The CoNiPO x @V 3% ‐Co 4 N/NF (+/−) electrolyzer utilizing the electrocatalyst as both anode and cathode demonstrates remarkable overall water‐splitting activity, requiring a cell potential of only 1.52 V at 10 mA cm −2 , 30 mV lower than that of the RuO 2 /NF (+)/20%‐Pt/C/NF (−) electrolyzer. Such impressive bifunctional activities can be attributed to abundant active sites, adjusted electronic structure, lower charge‐transfer resistance, enhanced electrochemically active surface area (ECSA), and surface‐ and volume‐confined electrocatalysis resulting from the synergistic effects of the crystalline V 3% ‐Co 4 N core and amorphous CoNiPO x shells boosting water splitting in alkaline media.

Electrostatic self-potentials of individual particles trapped at an oil–water interface were determined, and the effects of surface chemical nonuniformity on heterogeneous self-potentials and equilibrium microstructures were investigated. Direct measurement of the pair interactions and the self-potentials of polystyrene microspheres were performed using optical laser tweezers. The individual particles had different self-potentials even when they possessed the same surface functionalities. Atomic force microscopy measurements elucidated the relationship between nonuniform surface charge distribution and heterogeneity and magnitude of self-potentials. Monte Carlo simulations demonstrated that self-potential heterogeneity led to the formation of more melted microstructures that showed excellent consistency with experiments.