Enhanced charge separation and photocatalytic hydrogen evolution in carbonized-polymer-dot-coupled lead halide perovskites,Materials Horizons

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Enhanced charge separation and photocatalytic hydrogen evolution in carbonized-polymer-dot-coupled lead halide perovskites
Materials Horizons ( IF 12.2 ) Pub Date : 2020-07-28 , DOI: 10.1039/d0mh00955e
Yue Zhao _{1,

2,

3,

4,

5} , Qingsen Zeng _{1,

2,

3,

4,

5} , Yue Yu _{1,

2,

3,

4,

5} , Tanglue Feng _{1,

2,

3,

4,

5} , Yajie Zhao _{5,

6,

7,

8,

9} , Zidong Wang _{1,

2,

3,

4,

5} , Yi Li _{5,

6,

7,

8,

9} , Chongming Liu _{1,

2,

3,

4,

5} , Junjun Liu _{1,

2,

3,

4,

5} , Haotong Wei _{1,

2,

3,

4,

5} , Shoujun Zhu _{1,

2,

3,

4,

5} , Zhenhui Kang _{5,

6,

7,

8,

9} , Hao Zhang _{1,

2,

3,

4,

5} , Bai Yang _{1,

2,

3,

4,

5}

Affiliation

Metal halide perovskites are promising candidates as photocatalysts due to their uniquely outstanding photophysical properties; however, the catalytic efficiency is limited by severe charge recombination. Herein, we show that carbonized polymer dots (CPDs) can act as an efficient charge modulator to stabilize photo-generated carriers in methylamine lead triiodide (MAPbI₃) perovskites through ultra-fast hole transfer, and thus increase the rate of visible light-driven photocatalytic HI splitting 35-fold. The optimized CPD/MAPbI₃/Pt hybrid photocatalytic system exhibits an impressive H₂ evolution rate of 11 497 μmol h⁻¹ g⁻¹, a solar-to-hydrogen conversion efficiency of 2.15%, and an apparent quantum yield of 53.6% at 420 nm, which are among the highest values for metal halide perovskite photocatalysts. Moreover, the presented strategy of hole extraction via CPDs can be universally applied to improve the performance of previous electron-manipulated MAPbI₃-based photocatalytic systems. The easy-to-prepare and bandedge-tunable CPDs with excellent charge-transfer ability may bring new insights in developing high-performance perovskite photocatalysts.

中文翻译：

碳化聚合物点耦合卤化钙钛矿中增强的电荷分离和光催化氢的释放

金属卤化物钙钛矿因其独特的出色光物理性能而有望用作光催化剂。然而，催化效率受到严重的电荷复合的限制。在这里，我们表明碳化的聚合物点（CPDs）可以作为有效的电荷调节剂，通过超快速的空穴转移来稳定钙钛矿中甲胺三碘化铅（MAPbI ₃）中的光生载流子，从而提高可见光驱动率光催化HI分裂35倍。优化的CPD / MAPbI ₃ / Pt杂化光催化系统表现出令人印象深刻的H ₂析出速率11 497μmolh ^-1 g ^-1，其太阳能到氢的转换效率为2.15％，在420 nm下的表观量子产率为53.6％，是金属卤化物钙钛矿光催化剂的最高值。此外，所提出的经由CPD的空穴提取策略可以被普遍应用以改善先前基于电子操纵的MAPbI ₃的光催化系统的性能。具有优异的电荷转移能力的易于制备和能带边缘调节的CPD可能为开发高性能钙钛矿光催化剂带来新的见解。

更新日期：2020-10-05

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