{"title":"中性磷酸盐缓冲电解质中磷酸氢联产的自共电解","authors":"Heng Xu, Guanxing Xu, Lisong Chen, Jianlin Shi","doi":"10.1002/adma.202200058","DOIUrl":null,"url":null,"abstract":"<p>The spontaneous reaction between Zn and H<sub>2</sub>O is of critical importance and could plausibly be used to produce H<sub>2</sub> gas, especially under neutral conditions. However, this reaction has long been overlooked owing to its sluggish kinetics and Zn consumption. Herein, a unique self-co-electrolysis system (SCES) is reported, which uses a Zn anode, a CoP-based catalytic cathode, and a neutral phosphate buffer solution (PBS) as the electrolyte. In this SCES, Zn is not only a sacrificial anode but also an important precursor of high-value-added NaZnPO<sub>4</sub>. Additionally, the composition and phase structure of NaZnPO<sub>4</sub> can be well regulated. In this study, a high-performance N,Cu-CoP/carbon cloth (CC) catalyst is synthesized to catalyze the cathodic hydrogen evolution reaction (HER) at an especially low overpotential of 64.7 mV at 10 mA cm<sup>−</sup><sup>2</sup>. H<sub>2</sub> gas (13.7 mL cm<sup>−</sup><sup>2</sup> h<sup>−</sup><sup>1</sup>) and NaZnPO<sub>4</sub> (3.73 mg cm<sup>−</sup><sup>2</sup> h<sup>−</sup><sup>1</sup>) are obtained at the cathode and anode, respectively, in the N,Cu-CoP/CC||Zn SCES spontaneously. Moreover, the SCES has a favorable open-circuit voltage (OCV) of 0.79 V and a maximum power density of 1.83 mW cm<sup>−</sup><sup>2</sup>. Density functional theory (DFT) calculations are performed to elucidate the electronic structure and HER catalytic mechanism of the N and Cu co-doped CoP catalysts.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":null,"pages":null},"PeriodicalIF":27.4000,"publicationDate":"2022-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"8","resultStr":"{\"title\":\"Self-Co-Electrolysis for Co-Production of Phosphate and Hydrogen in Neutral Phosphate Buffer Electrolyte\",\"authors\":\"Heng Xu, Guanxing Xu, Lisong Chen, Jianlin Shi\",\"doi\":\"10.1002/adma.202200058\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>The spontaneous reaction between Zn and H<sub>2</sub>O is of critical importance and could plausibly be used to produce H<sub>2</sub> gas, especially under neutral conditions. However, this reaction has long been overlooked owing to its sluggish kinetics and Zn consumption. Herein, a unique self-co-electrolysis system (SCES) is reported, which uses a Zn anode, a CoP-based catalytic cathode, and a neutral phosphate buffer solution (PBS) as the electrolyte. In this SCES, Zn is not only a sacrificial anode but also an important precursor of high-value-added NaZnPO<sub>4</sub>. Additionally, the composition and phase structure of NaZnPO<sub>4</sub> can be well regulated. In this study, a high-performance N,Cu-CoP/carbon cloth (CC) catalyst is synthesized to catalyze the cathodic hydrogen evolution reaction (HER) at an especially low overpotential of 64.7 mV at 10 mA cm<sup>−</sup><sup>2</sup>. H<sub>2</sub> gas (13.7 mL cm<sup>−</sup><sup>2</sup> h<sup>−</sup><sup>1</sup>) and NaZnPO<sub>4</sub> (3.73 mg cm<sup>−</sup><sup>2</sup> h<sup>−</sup><sup>1</sup>) are obtained at the cathode and anode, respectively, in the N,Cu-CoP/CC||Zn SCES spontaneously. Moreover, the SCES has a favorable open-circuit voltage (OCV) of 0.79 V and a maximum power density of 1.83 mW cm<sup>−</sup><sup>2</sup>. Density functional theory (DFT) calculations are performed to elucidate the electronic structure and HER catalytic mechanism of the N and Cu co-doped CoP catalysts.</p>\",\"PeriodicalId\":114,\"journal\":{\"name\":\"Advanced Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":27.4000,\"publicationDate\":\"2022-03-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"8\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Advanced Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://onlinelibrary.wiley.com/doi/10.1002/adma.202200058\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Materials","FirstCategoryId":"88","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/adma.202200058","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 8
摘要
锌和水之间的自发反应是至关重要的,可以合理地用来产生氢气,特别是在中性条件下。然而,由于反应动力学缓慢和锌的消耗,该反应长期被忽视。本文报道了一种独特的自共电解系统(SCES),该系统使用Zn阳极,cop基催化阴极和中性磷酸盐缓冲溶液(PBS)作为电解质。在该SCES中,Zn不仅是牺牲阳极,而且是高附加值NaZnPO4的重要前驱体。此外,NaZnPO4的组成和相结构可以很好地调节。在本研究中,合成了一种高性能的N,Cu-CoP/碳布(CC)催化剂,用于催化阴极析氢反应(HER),其过电位为64.7 mV,电压为10 mA cm−2。在N,Cu-CoP/CC||Zn SCES中,阴极和阳极分别自发生成H2气体(13.7 mL cm−2 h−1)和NaZnPO4 (3.73 mg cm−2 h−1)。此外,ses具有0.79 V的良好开路电压(OCV)和1.83 mW cm−2的最大功率密度。采用密度泛函理论(DFT)分析了N、Cu共掺CoP催化剂的电子结构和HER催化机理。
Self-Co-Electrolysis for Co-Production of Phosphate and Hydrogen in Neutral Phosphate Buffer Electrolyte
The spontaneous reaction between Zn and H2O is of critical importance and could plausibly be used to produce H2 gas, especially under neutral conditions. However, this reaction has long been overlooked owing to its sluggish kinetics and Zn consumption. Herein, a unique self-co-electrolysis system (SCES) is reported, which uses a Zn anode, a CoP-based catalytic cathode, and a neutral phosphate buffer solution (PBS) as the electrolyte. In this SCES, Zn is not only a sacrificial anode but also an important precursor of high-value-added NaZnPO4. Additionally, the composition and phase structure of NaZnPO4 can be well regulated. In this study, a high-performance N,Cu-CoP/carbon cloth (CC) catalyst is synthesized to catalyze the cathodic hydrogen evolution reaction (HER) at an especially low overpotential of 64.7 mV at 10 mA cm−2. H2 gas (13.7 mL cm−2 h−1) and NaZnPO4 (3.73 mg cm−2 h−1) are obtained at the cathode and anode, respectively, in the N,Cu-CoP/CC||Zn SCES spontaneously. Moreover, the SCES has a favorable open-circuit voltage (OCV) of 0.79 V and a maximum power density of 1.83 mW cm−2. Density functional theory (DFT) calculations are performed to elucidate the electronic structure and HER catalytic mechanism of the N and Cu co-doped CoP catalysts.
期刊介绍:
Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.