Stable and high-yield hydrogen peroxide electrosynthesis from seawater

IF 27.1 1区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES
Chaoqi Zhang, Pengyue Shan, Yingying Zou, Tong Bao, Xinchan Zhang, Zhijie Li, Yunying Wang, Guangfeng Wei, Chao Liu, Chengzhong Yu
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Abstract

Electrocatalytic two-electron oxygen reduction reaction (2e− ORR) in seawater offers a sustainable route for hydrogen peroxide (H2O2) production. However, due to the high concentration of Cl− ions and competitive 4e− ORR, there is a lack of efficient and long-term stable seawater electrocatalysts. Here we report a high-performance electrocatalyst design based on NiPS3 nanosheets enabling efficient H2O2 production from seawater. Specifically, the NiPS3 nanosheets deliver a 2e− ORR selectivity of ∼98%, a H2O2 yield of 6.0 mol gcat−1 h−1 and robust stability for over 1,000 h in simulated seawater. Underlying the exciting performance is the synergy of the S2−, Ni2+ and P4+ sites where the octahedral S2− skeleton repels Cl− ions, the Ni2+ sites enable the modest binding strength of *OOH intermediate, and the P4+ sites interact with H2O to trigger the protonation of proximal O atom of *OOH. The seawater electrocatalysis system also allows for scalable synthesis of solid H2O2, tandem oxidation reaction of biomass to organic acid and direct use of the produced H2O2 as a sterilizing agent. Once integrated with photovoltaics, the solar-powered electrolysis device can operate in real seawater. Our findings pave the way for sustainable conversion of seawater into value-added products. Hydrogen peroxide (H2O2) is a green oxidant with diverse applications. Aided by a nickel phosphorus trisulfide nanosheet electrocatalyst, this work shows a sustainable synthetic route to produce H2O2 from seawater with high yield and impressive stability.

Abstract Image

稳定、高产的海水电合成过氧化氢
海水中电催化双电子氧还原反应(2e−ORR)为生产过氧化氢(H2O2)提供了一条可持续的途径。然而,由于Cl−离子的高浓度和竞争性的4e−ORR,缺乏高效、长期稳定的海水电催化剂。在这里,我们报道了一种基于NiPS3纳米片的高性能电催化剂设计,可以从海水中高效地生产H2O2。具体来说,NiPS3纳米片的2e - ORR选择性为~ 98%,H2O2产率为6.0 mol gcat - 1 h - 1,并且在模拟海水中具有超过1000小时的稳定性。这一令人兴奋的表现背后是S2 -, Ni2+和P4+位点的协同作用,其中八面体S2 -骨架排斥Cl -离子,Ni2+位点使*OOH中间体具有适度的结合强度,P4+位点与H2O相互作用触发*OOH近端O原子的质子化。海水电催化系统还可以大规模合成固体H2O2,将生物质串联氧化成有机酸,并直接使用生成的H2O2作为灭菌剂。一旦与光伏集成,太阳能电解装置就可以在真正的海水中运行。我们的发现为可持续地将海水转化为增值产品铺平了道路。过氧化氢(H2O2)是一种具有多种用途的绿色氧化剂。在三硫化镍磷纳米片电催化剂的帮助下,这项工作展示了一种可持续的从海水中生产H2O2的合成途径,具有高产率和令人印象深刻的稳定性。
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来源期刊
Nature Sustainability
Nature Sustainability Energy-Renewable Energy, Sustainability and the Environment
CiteScore
41.90
自引率
1.10%
发文量
159
期刊介绍: Nature Sustainability aims to facilitate cross-disciplinary dialogues and bring together research fields that contribute to understanding how we organize our lives in a finite world and the impacts of our actions. Nature Sustainability will not only publish fundamental research but also significant investigations into policies and solutions for ensuring human well-being now and in the future.Its ultimate goal is to address the greatest challenges of our time.
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