Efficient solar steam generation and concurrent salt harvesting from saline water were achieved with both continuous operation and long-term stability.
The
synthesis of hydrogen peroxide (H2O2)
from H2O and O2 by metal-free photocatalysts
(e.g., graphitic carbon nitride, C3N4) is a
potentially promising approach to generate H2O2. However, the photocatalytic H2O2 generation
activity of the pristine C3N4 in pure H2O is poor due to unpropitious rapid charge recombination and
unfavorable selectivity. Herein, we report a facile method to boost
the photocatalytic H2O2 production by grafting
cationic polyethylenimine (PEI) molecules onto C3N4. Experimental results and density functional theory (DFT)
calculations demonstrate PEI can tune the local electronic environment
of C3N4. The unique intermolecular electronic
interaction in PEI/C3N4 not only improves the
electron–hole separation but also promotes the two-electron
O2 reduction to H2O2 via the sequential
two-step single-electron reduction route. With the synergy of improved
charge separation and high selectivity of two-electron O2 reduction, PEI/C3N4 exhibits an unexpectedly
high H2O2 generation activity of 208.1 μmol
g–1 h–1, which is 25-fold higher
than that of pristine C3N4. This study establishes
a paradigm of tuning the electronic property of C3N4 via functional molecules for boosted photocatalysis activity
and selectivity.
energy storage and conversion devices, [26][27][28] as outlined in recent reviews (Figure 1, left). [29] Behind these applications lie a fundamental question: how water and ion transport are controlled in the laminar structure to obtain desired selectivity. A comprehensive summary of structure-transport relation is thereby imperative to understand and optimize membrane selective performance, but is so far lacking. In such context, our review aims to fill this gap by discussing: 1) how 2D materials with specific physicochemical features are assembled into laminar membranes; 2) most importantly, how membrane structure, and its response to external impacts, can tune mass transport (herein, water and ions); 3) how these transport mechanisms translate into selectivity in applications, and into future design of high-performance laminar membranes. Unsolved problems and emerging challenges around these topics are then concluded. We note that the knowledge summarized here can also, at least partly, assist the understanding of the selective gas, liquid, and micromolecule transport through laminar membranes, which are gaining considerable attention as well. [30][31][32] Transition Metal Carbides and/or Nitrides (MXene): MXene nanosheets are etched and delaminated from parent bulk MAX to M n+1 X n T x (e.g., Ti 3 C 2 T x ), and have thus several atom sublayers. [39] While M and X are early transition metal
Owing to the rich porosity and uniform pore size, metal-organic frameworks (MOFs) offer substantial advantages over other materials for the precise and fast membrane separation. However, achieving ultrathin water-stable MOF membranes remains a great challenge. Here, we first report the successful exfoliation of two-dimensional (2D) monolayer aluminum tetra-(4-carboxyphenyl) porphyrin framework (termed Al-MOF) nanosheets. Ultrathin water-stable Al-MOF membranes are assembled by using the exfoliated nanosheets as building blocks. While achieving a water flux of up to 2.2 mol m−2 hour−1 bar−1, the obtained 2D Al-MOF laminar membranes exhibit rejection rates of nearly 100% on investigated inorganic ions. The simulation results confirm that intrinsic nanopores of the Al-MOF nanosheets domain the ion/water separation, and the vertically aligned aperture channels are the main transport pathways for water molecules.
Graphene-based laminar membranes open new avenues for water treatment; in particular, reduced graphene oxide (rGO) membranes with high stability in aqueous solutions are gaining increased attention for desalination. However, the low water permeability of these membranes significantly limits their applications. In this study, the water permeability of thermally reduced GO membrane was increased by a factor of 26 times by creating in-plane nanopores with an average diameter of ∼3 nm and a high density of 2.89 × 10 15 m −2 via H 2 O 2 oxidation. These in-plane nanopores provide additional transport channels and shorten the transport distance for water molecules. Meanwhile, salt rejection of this membrane is dominated by both the Donnan effect and the size exclusion of the interspaces. Besides, the water permeability and salt rejection of the thermally reduced nanoporous GO membrane can also be simply tuned by adjusting the thermal treatment time and membrane thickness. Additionally, the fabricated membrane exhibited a relatively stable rejection of Na 2 SO 4 during the long-term testing. This work demonstrates a novel and effective strategy for fabricating high-performance laminar rGO membranes for desalination applications.
Building bridges: Two arylimido derivatives of hexamolybdate, containing unprecedented bridging imido ligands, have been synthesized and structurally characterized. Their 1H NMR and UV/Vis spectra distinguish them from related terminally coordinated derivatives. Such compounds extend the range of organoimido polyoxometalate coordination chemistry, providing insight into the mechanism of oxo metathesis in the Lindqvist polymolybdate.
Benefiting from vast solar energy access and high energy conversion efficiency, solar-driven interfacial water evaporation has shown great potential in critical separation processes such as desalination and waste brine treatment....
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