Re-usable Cd_(0.9)Zn_(0.1)S-ZnO@C/PVDF piezo-photocatalytic film with exceptional hydrogen evolution capability triggered by the synergetic advantages of piezoelectricity and S-Scheme heterojunction

Piezoelectric materials have advantages of fine-tuning photocatalytic performance through harvesting mechanical energy and open a new avenue in facilitating green catalytic reaction.Herein,polyvinylidene fluoride(PVDF),a flexible piezoelectric material,was introduced to synthesize a novel Cd_(0.9)Zn_(0.1)S-ZnO@C/PVDF(CZS-ZO@C/PVDF)piezo-photocatalytic film by spin coating and immersion phase conversion method.Benefiting from the piezoelectricity of PVDF and the internal electric field(IEF)of CZS-ZO@C Step-scheme(S-Scheme)heterojunction,CZS-ZO@C/PVDF was able to induce a hydrogen generation rate of 34.9 mmol g^(−1)h^(−1)activated by ultrasound and visible light(U-L),which is∼17.5 times of Cd_(0.9)Zn_(0.1)S/PVDF(CZS/PVDF)and∼7.4 times of the photocatalysis rate activated by visible light only(L).Piezoelectric measurements and COMSOL simulation illustrated the excellent piezoelectricity of CZS-ZO@C/PVDF film,which exhibits a piezoelectric coefficient(d33)of 9.9 pm V−1 and a piezoelectric potential of 874 mV(under 0.5 MPa).The reaction mechanism for the exceptional piezo-photocatalytic performance was finally disclosed through density functional theory(DFT)calculation and electrochemical tests.This study enriches the application scope of piezoelectric materials in sustainable energy catalysis and provides a new direction to develop efficient piezoelectric photocatalysts.

Rational construction of CuFe_(2)O_(4)@C/Cd_(0.9)Zn_(0.1)S S-scheme heterojunction photocatalyst for extraordinary photothermal-assisted photocatalytic H_(2) evolution

Rational design of photocatalyst to maximize the use of sunlight is one of the issues to be solved in photocatalysis technology.In this study,the CuFe_(2)O_(4)@C/Cd_(0.9)Zn_(0.1)S(CFO@C/CZS)S-scheme photocatalyst with photothermal effect was synthesized by ultrasonic self-assembly combined with calcination.The dark CFO@C absorbed visible light and partly converted into heat to promote the hydrogen evolution reaction.The presence of heterojunctions inhibited the photogenerated electron-hole recombination.The graphite-carbon layer provided a stable channel for electron transfer,and the presence of magnetic CFO made recycle easier.Under the action of photothermal assistance and heterojunction,the hydrogen evolution rate of the optimal CFO@C/CZS was 80.79 mmol g^(-1) h^(-1),which was 2.55 times and 260.61 times of that of pure CZS and CFO@C,respectively.Notably,the composite samples also exhibit excellent stability and a wide range of environmental adaptability.Through experimental tests and first-principles simulation calculation methods,the plausible mechanism of photoactivity enhancement was proposed.This work provided a feasible strategy of photothermal assistance for the development of heterojunction photocatalysts with distinctive hydrogen evolution.

双层膦氧化物分子修饰制备高效的大面积纯蓝光钙钛矿量子点发光二极管

蓝光卤素钙钛矿发光二极管(LED)由于其高色纯度和全色钙钛矿LED发展需求目前受到越来越多的关注.通过钝化卤素钙钛矿中的缺陷来提高LED性能是主要研究方向,然而,用于有效钝化混合卤素蓝光钙钛矿并获得性能优异、光谱稳定的纯蓝光LED方法还很有限.本文开发了一种使用含有膦氧基团的双层有机分子对混合卤素蓝光钙钛矿量子点进行固相修饰,不仅有效提高了量子点薄膜的发光性能,而且有效改善了LED的电荷平衡,显著提高了器件性能,获得了最大外量子效率为4.87%的纯蓝光LED(469 nm).作者发现双层膦氧分子与量子点之间可以发生强相互作用,从而有效钝化量子点,并有助于获得大面积单层钙钛矿量子点薄膜.其中,发光面积为64 mm2,波长为469 nm的LED最大外量子效率为3.91%.本文所述策略有助于推动性能优异的大面积钙钛矿量子点光电器件开发.

SnFe_(2)O_(4)/ZnIn_(2)S_(4)/PVDF piezophotocatalyst with improved photocatalytic hydrogen production by synergetic effects of heterojunction and piezoelectricity

The polarized electric field inside piezoelectric materials has been proven to be a promising technique to boost photogenerated charge separation.Herein,a novel flexible SnFe_(2)O_(4)/ZnIn_(2)S_(4)/polyvinylidene fluoride((CH2CF2)_(n),PVDF)(P-SZ)film piezophotocatalyst was successfully synthesized by combining PVDF,an organic piezoelectric material,with a SnFe_(2)O_(4)/ZnIn_(2)S_(4)(SFO/ZIS)type II heterojunction photocatalyst.The hydrogen evolution rate of SFO/ZIS heterojunction with a SFO content of 5%is about 846.79μmol·h^(−1)·g^(−1),which is 3.6 times that of pristine ZIS.Furthermore,after being combined with PVDF,the optimum hydrogen evolution rate of P-SZ is about 1652.7μmol·h^(−1)·g^(−1)in the presence of ultrasound,which exceeds that of 5%SFO/ZIS by an approximate factor of 2.0.Based on experimental results,the mechanism of the improved photocatalytic performance of P-SZ was proposed on the basis of the piezoelectric field in PVDF and the formed heterojunction between SFO and ZIS,which effectively boosted the separation of photoinduced charges.This work provides an efficient strategy for multi-path collection and utilization of natural solar and vibrational energy to enhance photoactivity.

High-performance all-solution-processed inverted quantum dot light-emitting diodes enabled by water treatment

All-solution-processed inverted quantum dot(QD)light-emitting diodes(QLEDs)with transparent bottom cathodes can be directly connected to the n-type thin-film transistors,offering a feasible solution for low-cost active matrix-driven QD displays.However,the subsequent solution-deposition of the hole-transporting layer destroys the underneath QD films,resulting in largely deteriorated device performance.Various strategies have been implemented to prevent QD film from dissolution,but all at a heavy cost of device performance suffering from either reduced efficiency or increased driving voltage.Here,a facile and effective water-treatment approach for QD film to fabricate inverted QLEDs through all solution processing is reported.The water treatment substitutes the long-chain oleate ligands with hydroxyl groups,resulting in significantly improved non-polar solvent resistance of the QD films.Importantly,the QD films reserve their excellent photoluminescence efficiency after water treatment.With the water-treated QD film as the emissive layer,all-solution-processed inverted red QLED with a peak external quantum efficiency of 19.6%,a turn-on voltage of 1.8 V,and a T50 operational lifetime of 150,000 h at 100 cd·m^(-2) was achieved.Furthermore,efficient and low-voltage-driven green and blue QLEDs can also be prepared with this method.This work provides a feasible strategy for the fabrication of high-performance all-solution-processed inverted QLEDs,paving the way toward achieving QLEDs by all ink-jet printing.