Photocatalytic H2 evolution coupled with organic transformation provides a new avenue to cooperatively produce clean fuels and fine chemicals, enabling a more efficient conversion of solar energy. Here, a novel two-dimensional (2D) heterostructure of ultrathin ZnIn2S4 nanosheets decorated with amorphous nickel boride (Ni x -B) is prepared for simultaneous photocatalytic anaerobic H2 generation and aromatic aldehydes production. This ZnIn2S4/Ni x -B catalyst elaborately combines the ultrathin structure advantage of the ZnIn2S4 semiconductor and the cocatalytic function of Ni x -B. A high H2 production rate of 8.9 mmol h–1 g–1 is delivered over the optimal ZnIn2S4/Ni x -B with a stoichiometric production of benzaldehyde, which is about 22 times higher than ZnIn2S4. Especially, the H2 evolution rate is much higher than the value (2.8 mmol h–1 g–1) of the traditional photocatalytic half reaction of H2 production with triethanolamine as a sacrificial agent. The apparent quantum yield reaches 24% at 420 nm, representing an advanced photocatalyst system. Moreover, compared with traditional sulfide, hydroxide, and even noble metal modified ZnIn2S4/M counterparts (M = NiS, Ni­(OH)2, Pt), the ZnIn2S4/Ni x -B also maintains markedly higher photocatalytic activity, showing a highly efficient and economical advantage of the Ni x -B cocatalyst. This work sheds light on the exploration of 2D ultrathin semiconductors decorated with novel transition metal boride cocatalyst for efficient photocatalytic organic transformation integrated with solar fuel production.

In the past two decades, mussels have inspired the design of novel adhesives that can be used underwater, since they secrete a super-strong mucus (mussel adhesion proteins, MAPs) that keeps them firmly attached to the surface of the reef beneath the sea, braving wind, and waves. [3] Structure-function relationship studies on MAPs have disclosed the sophisticated mechanisms for adhesion; nevertheless, the key factor is the catechol containing 3, 4-dihydroxyphenylalanine residue, and many biomimetic adhesives were designed based on this key structure. [4] This work can be traced back to Messersmith's first publication for reversible wet/ dry adhesives using catechol-containing poly(acrylamide-acrylate) coated nanofabricated polymer pillars. [5] After that, the design of mussel-inspired adhesives is under fast growth, and many polymers conjugated with catechol moieties have been reported. Most of them were focused on the bio-adhesives that can be used in dry and humid environments, and some of them even exceeded the adhesive properties of natural mussels. [6] In contrast, the studies on the mussel-inspired adhesives that can be directly used in underwater conditions are lagged behind, and only handful of cases have been reported. For instance, Joy et al. synthesized a mussel-inspired self-coacervating polyester, which showing rapidly adhere to substrates submerged underwater and exhibiting an adhesion strength of ≈100 kPa when cured under UV-A irradiation for 10 min under underwater conditions. [7] Zhou et al. synthesized poly(dopamine-alt-2,2-bis-(4-glycidyloxyphenyl) propane) via epoxy-amino click chemistry, which exhibited a bonding strength up to 1.1 MPa on glass substrates at an underseawater condition after curing in artificial seawater at room temperature for a week. [8] Liu et al. reported a hyperbranched polymer with a hydrophobic backbone and hydrophilic adhesive catechol side branches, which exhibited a bonding strength up to 0.4 MPa on iron sheets after curing in water for 12 h. [9] More recently, poly(catechol-styrene) developed by Wilker's group displayed underwater bonding up to 3.1 MPa when curd at room temperature for 24 h. [10] We also showed that when catechol was grafted onto polyvinylpyrrolidone, the resulting polymer showed an underwater bonding strength at 1.1 MPa at the same curing time. [11] These reported adhesives generally take a long time to reach the best underwater bonding strength but only exhibit relatively low bonding strength in a short curing time, How to realize fast and strong underwater adhesion has gained much attention recently. Although some mussel-inspired adhesives that can be cured underwater have been reported, reports on underwater adhesion with both high bonding strength and rapid curing capability are still rare. Furthermore, organic solvents are generally utilized in these adhesives, which are ecounfriendly. Here, by taking advantages of the strong underwater adhesion capability of catecholic groups in mussel adhesion proteins (MAPs) and the fast curing capability of...

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