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APPLIED CATALYSIS B-ENVIRONMENTAL · 2023 · IF 22.1

Construction atomic-level N-P charge transfer channel for boosted CO2 photoreduction

Zheyang Liu,Jianli Liang,Qianqian Song,Yang Li,Zhiquan Zhang,Min Zhou,Wei Wei,Hui Xu,Chun-Sing Lee,Huaming Li,Zhifeng Jiang

Efficient conversion of CO 2 to high value-added chemical products is a promising strategy for achieving carbon neutrality . Although the photocatalyst technique has been made widespread researched, highly efficient photoreduction CO 2 with metal-free photocatalysts remains a challenge. Herein, we report a zero-dimensional black phosphorus quantum dots (BPQDs)-decorated one-dimensional carbon nitride nanotubes (CNNT) photocatalyst that reduces CO 2 to CO with a rate of 44.6 μmol g –1 h –1 , which is better than the similar photocatalysts and pristine carbon nitride nanotubes . Synchrotron radiation XAFS measurements substantiate the construction of N-P electron transfer channels within BPQDs and CNNT. Time-resolved PL spectrum demonstrates the faster separated electron hole pairs . In situ irradiated X-ray photoelectron spectroscopy confirms the photogenerated-electron flow trend and the active site of photocatalytic reaction. Moreover, the main intermediate *COOH is verified by in situ FT-IR characterization which is corresponding to the previous research. The construction of atomic-level N-P charge transfer channel efficiently facilitates the charge transfer and accelerates the catalytic rate. This work provides a novel insight into the design of BPQDs-anchoring heterostructures for photocatalytic CO 2 reduction.

研究领域: 光催化化学 · 纳米材料科学 · 环境能源技术
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Nature Catalysis · 2023 ·Vol. 6 ·期 2 ·174-184 · IF 37.8

Optimizing the p charge of S in p-block metal sulfides for sulfur reduction electrocatalysis

Hua Wuxing,Shang Tongxin,Li Huan,Sun Yafei,Guo Yong,Xia Jingyi,Geng Chuannan,Hu Zhonghao,Peng Linkai,Han Zhiyuan,Zhang Chen,Lv Wei,Wan Ying

Understanding sulfur conversion chemistry is key to the development of sulfur-based high-energy-density batteries. However, unclear relationships between the electronic structure of the catalyst and its activity are the major problem. Here, we provide a direct correlation between the p electron gain of S in p -block metal sulfides and the apparent activation energies ( E a ) for the sulfur reduction reaction (SRR), in particular, Li 2 S n to Li 2 S conversion, which is the rate-determining step of the SRR. The maximum p charge occurs in bismuth sulfide and results in the lowest E a and a high SRR rate in the cathode. Li–S batteries with the Bi 2 S 3 catalyst work steadily at a high rate of 5.0C with a high-capacity retention of ~85% after 500 cycles. A high areal capacity of ~21.9 mAh cm −2 was obtained under a high sulfur loading of 17.6 mg cm −2 but a low electrolyte/sulfur ratio of 7.5 μl mg −1 .

研究领域: 材料科学 · 电化学 · 电池技术 · 催化
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