Tian Zhangliu, Wang Meng, Chen Ganwen, Chen Jie, Da Yumin, Zhang Hanqian, Jiang Rui, Xiao Yukun, Cui Baihua, Jiang Chonglai, Ding Yishui, Yang Jinlin, Sun Zejun, Han Cheng, Chen Wei
Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543, Singapore.
State Key Laboratory of Radio Frequency Heterogeneous Integration, and International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education, Institute of Microscale Optoelectronics, Shenzhen University, Shenzhen, 518060, China.
Angew Chem Int Ed Engl. 2025 Jan 10;64(2):e202414209. doi: 10.1002/anie.202414209. Epub 2024 Nov 7.
Photoelectrochemical water splitting offers a promising approach for carbon neutrality, but its commercial prospects are still hampered by a lack of efficient and stable photoelectrodes with earth-abundant materials. Here, we report a strategy to construct an efficient photoanode with a coaxial nanobelt structure, comprising a buried-ZrS/ZrOS n-p junction, for photoelectrochemical water splitting. The p-type ZrOS layer, formed on the surface of the n-type ZrS nanobelt through a pulsed-ozone-treatment method, acts as a hole collection layer for hole extraction and a protective layer to shield the photoanode from photocorrosion. The resulting ZrS/ZrOS photoanode exhibits light harvesting with good photo-to-current efficiencies across the whole visible region to over 650 nm. By further employing NiOOH/FeOOH as the oxygen evolution reaction cocatalyst, the ZrS/ZrOS/NiOOH/FeOOH photoanode yields a photocurrent density of ~9.3 mA cm at 1.23 V versus the reversible hydrogen electrode with an applied bias photon-to-current efficiency of ~3.2 % under simulated sunlight irradiation in an alkaline solution (pH=13.6). The conformal ZrOS layer enables ZrS/ZrOS/NiOOH/FeOOH photoanode operation over 1000 hours in an alkaline solution without obvious performance degradation. This study, offering a promising approach to fabricate efficient and durable photoelectrodes with earth-abundant materials, advances the frontiers of photoelectrochemical water splitting.
光电化学水分解为实现碳中和提供了一种很有前景的方法，但其商业前景仍受到缺乏采用储量丰富的材料制成的高效且稳定的光电极的阻碍。在此，我们报告了一种构建具有同轴纳米带结构的高效光阳极的策略，该结构包含用于光电化学水分解的掩埋式ZrS/ZrOS n-p结。通过脉冲臭氧处理方法在n型ZrS纳米带表面形成的p型ZrOS层，作为空穴收集层用于空穴提取，并作为保护层以保护光阳极免受光腐蚀。所得的ZrS/ZrOS光阳极在整个可见光区域至超过650 nm的范围内均表现出良好的光电流转换效率的光捕获能力。通过进一步采用NiOOH/FeOOH作为析氧反应助催化剂，在碱性溶液（pH = 13.6）中模拟太阳光照射下，ZrS/ZrOS/NiOOH/FeOOH光阳极在相对于可逆氢电极1.23 V时产生的光电流密度约为9.3 mA cm，施加偏压下的光子到电流效率约为3.2 %。保形的ZrOS层使ZrS/ZrOS/NiOOH/FeOOH光阳极在碱性溶液中能够运行超过1000小时而没有明显的性能下降。这项研究为使用储量丰富的材料制造高效且耐用的光电极提供了一种很有前景的方法，推动了光电化学水分解的前沿发展。
