State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310014, P. R. China.
Small. 2023 Jun;19(25):e2207852. doi: 10.1002/smll.202207852. Epub 2023 Mar 17.
The utilization of thermodynamically favorable sulfur oxidation reaction (SOR) as an alternative to sluggish oxygen evolution reaction is a promising technology for low-energy H production while degrading the sulfur source from wastewater. Herein, amorphous/crystalline S-doped Pd nanosheet arrays on nickel foam (a/c S-Pd NSA/NF) is prepared by S-doping crystalline Pd NSA/NF. Owing to the ultrathin amorphous nanosheet structure and the incorporation of S atoms, the a/c S-Pd NSA/NF provides a large number of active sitesand the optimized electronic structure, while exhibiting outstanding electrocatalytic activity in hydrogen evolution reaction (HER) and SOR. Therefore, the coupling system consisting of SOR-assisted HER can reach a current density of 100 mA cm at 0.642 V lower than conventional electrolytic water by 1.257 V, greatly reducing energy consumption. In addition, a/c S-Pd NSA/NF can generate H over a long period of time while degrading S in water to the value-added sulfur powder, thus further reducing the cost of H production. This work proposes an attractive strategy for the construction of an advanced electrocatalyst for H production and utilization of toxic sulfide wastewater by combining S-doping induced partial amorphization and ultrathin metal nanosheet arrays.
利用热力学有利的硫氧化反应 (SOR) 替代缓慢的氧气析出反应，是一种在降解废水中硫源的同时，低能耗生产氢气的有前途的技术。在此，通过在结晶 Pd NSA/NF 上掺杂 S，制备了非晶/结晶 S 掺杂 Pd 纳米片阵列 (a/c S-Pd NSA/NF)。由于超薄的非晶纳米片结构和 S 原子的掺入，a/c S-Pd NSA/NF 提供了大量的活性位点和优化的电子结构，同时在析氢反应 (HER) 和 SOR 中表现出出色的电催化活性。因此，由 SOR 辅助 HER 组成的耦合系统可以达到 100 mA cm 的电流密度，比传统水电解低 0.642 V，降低了 1.257 V，大大降低了能耗。此外，a/c S-Pd NSA/NF 可以在很长一段时间内产生 H，同时将水中的 S 降解为增值的硫粉，从而进一步降低 H 生产的成本。这项工作提出了一种有吸引力的策略，通过 S 掺杂诱导的部分非晶化和超薄金属纳米片阵列，构建用于 H 生产和利用有毒硫化物废水的先进电催化剂。
