High-current
density (≥1 A cm–2) is a
critical factor for large-scale industrial application of water-splitting
electrocatalysts, especially seawater-splitting. However, it still
remains a great challenge to reach high-current density due to the
lack of active and stable intrinsic catalytic active sites in catalysts.
Herein, we report an original three-dimensional self-supporting graphdiyne/molybdenum
oxide (GDY/MoO3) material for efficient hydrogen evolution
reaction via a rational design of “sp C–O–Mo
hybridization” on the interface. The “sp C–O–Mo
hybridization” creates new intrinsic catalytic active sites
(nonoxygen vacancy sites) and increases the amount of active sites
(eight times higher than pure MoO3). The “sp C–O–Mo
hybridization” facilitates charge transfer and boosts the dissociation
process of H2O molecules, leading to outstanding HER activity
with high-current density (>1.2 A cm–2) in alkaline
electrolyte and a decent activity and stability in natural seawater.
Our results show that high-current density electrocatalysts can be
achieved by interfacial chemical bond engineering, three-dimensional
structure design, and hydrophilicity optimization.
Conjugated polyacetylenes having pendant fullerene and/or porphyrin groups were prepared
by copolymerization in the presence of [Rh(nbd)Cl]2−NEt3 in CHCl3. The photochemical and electrochemical properties of the polymers were studied by UV−vis spectroscopy and voltammetry. The photoinduced
charge-transfer properties of the monolayer films were also measured by a three-electrode cell technique.
More importantly, poly(1a
0.2-co-5
0.8) shows a high capacity to form a photoinduced charge-separated state
and to produce steady and prompt photocurrent at the irradiation of 21.2 mW cm-2 white light. We
estimate an aerobic IPCE value of 0.15% for a true monolayer coverage of poly(1a
0.2-co-5
0.8) at its peak
absorption around 440 nm (the maximum of the Soret band).
The ladder-type nonacyclic arene (bis(thieno[3,2b]thieno)cyclopentafluorene (BTTF)) has been designed and synthesized through fusing thienothiophenes with the fluorene core from the synthon of dimethyl9 ,9-dioctyl-2,7-bis(thieno[3,2-b]thiophen-2-yl)fluorene-3,6-dicarboxylate. With BTTF as the central donor unit, an ovel acceptor-donor-acceptor (A-D-A) type non-fullerene small-molecule acceptor (BTTFIC)w as prepared with 1,1-dicyanomethylene-3-indanones (IC) as the peripheral acceptor units.T he energy level of the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) of BTTFIC locate at À5.56 and À3.95 eV,r espectively,p resentingalow opticalb and gap of 1.58 eV.E ncouragingly,p olymer solar cells based on the blends of BTTFIC with both the representative wide-andl ow-bandgap polymer donors (PBDB-T, 1.82 eV.P TB7-Th, 1.58 eV) offer powerc onversion efficiencies over 8% (8.78 AE 0.18 %f or PBDB-T:BTTFIC and 8.18 AE 0.29 % for PTB7-Th:BTTFIC). These results highlightt he advantage of ladder-type BTTF on the preparation of nonfullerene acceptors with extended conjugated backbones.[a] X.Scheme2.Synthesis of ladder-typenonacyclic arene of bis(thieno[3,2-b]thieno)cyclopentafluorene (BTTF)and non-fullerene acceptorofBTTFIC.
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