AgPd3/2D-CdS 光催化剂：AgPd3 协同催化剂的功能以及在可见光下增强的光催化制氢性能

IF 8.3 2区工程技术 Q1 CHEMISTRY, PHYSICAL

International Journal of Hydrogen Energy Pub Date : 2025-03-13 DOI:10.1016/j.ijhydene.2025.03.157

Yangbo Ma , Miao Fa , Yihui Zhang , Liuying Xiong , Xiying Li , Shuaishuai Zhou , Wei Chen , Liqun Mao

{"title":"AgPd3/2D-CdS 光催化剂：AgPd3 协同催化剂的功能以及在可见光下增强的光催化制氢性能","authors":"Yangbo Ma , Miao Fa , Yihui Zhang , Liuying Xiong , Xiying Li , Shuaishuai Zhou , Wei Chen , Liqun Mao","doi":"10.1016/j.ijhydene.2025.03.157","DOIUrl":null,"url":null,"abstract":"<div><div>Precious metals loading strategy is an effective method to increase the reactivity of CdS based photocatalysts for hydrogen evolution from water splitting under visible light. The key problem of such strategy is the affecting mechanism, which determined by the composition, species and structure of the loaded metals. In this study, AgPd bimetallic nanoclusters (AgxPdy) were prepared and then loaded onto the surface of snowflake-like CdS and the affecting mechanism was qualitatively and quantatively investigated through both instrumental analysis and computational method. The composition and structure of synthesized samples were examined through XRD, TEM, and XPS, by which the successful synthesis of AgPd bimetallic nanocluster alloys with an average particle size of approximately 3 nm were confirmed. Further, the hydrogen evolution performance of AgxPdy/CdS was tested under visible light and the prepared AgPd3/CdS achieved a hydrogen evolution rate of 73.93 mmol h−1 g−1, which is a 28 % improvement over Pd/CdS and a 381 % improvement over CdS, with an AQY of 44.68 % at 420 nm. The photoelectrochemical tests (LSV, I-T, EIS, PL, and TR-PL), ESR, and TRPL were applied to qualitatively demonstrate the function of AgxPdy nano-cocatalyst, and the testing results indicated that the cocatalyst significantly enhances the separation and transfer efficiency of photoinduced electrons, while further lowering the hydrogen evolution reaction energy barrier. Based on that, affecting mechanism was further determined through DFT simulation quantitatively. The prediction results indicated that the unique nanoclusters structure of AgPd3 contribute with the high work function and low d band center position increase the transfer efficiency of the photoinduced charge carriers. This study quantitatively revealed the relationship among compostion, structure and reactivity of the photocatalysts, provided an method to investigate the affecting mechanism of bimetallic hydrogen evolution photocatalysts and contributed to the advancement of renewable energy development.</div></div>","PeriodicalId":337,"journal":{"name":"International Journal of Hydrogen Energy","volume":"116 ","pages":"Pages 378-388"},"PeriodicalIF":8.3000,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"A AgPd3/2D-CdS photocatalyst: The function of AgPd3 cocatalyst, and the enhanced photocatalytic hydrogen generation property under visible light\",\"authors\":\"Yangbo Ma , Miao Fa , Yihui Zhang , Liuying Xiong , Xiying Li , Shuaishuai Zhou , Wei Chen , Liqun Mao\",\"doi\":\"10.1016/j.ijhydene.2025.03.157\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Precious metals loading strategy is an effective method to increase the reactivity of CdS based photocatalysts for hydrogen evolution from water splitting under visible light. The key problem of such strategy is the affecting mechanism, which determined by the composition, species and structure of the loaded metals. In this study, AgPd bimetallic nanoclusters (AgxPdy) were prepared and then loaded onto the surface of snowflake-like CdS and the affecting mechanism was qualitatively and quantatively investigated through both instrumental analysis and computational method. The composition and structure of synthesized samples were examined through XRD, TEM, and XPS, by which the successful synthesis of AgPd bimetallic nanocluster alloys with an average particle size of approximately 3 nm were confirmed. Further, the hydrogen evolution performance of AgxPdy/CdS was tested under visible light and the prepared AgPd3/CdS achieved a hydrogen evolution rate of 73.93 mmol h−1 g−1, which is a 28 % improvement over Pd/CdS and a 381 % improvement over CdS, with an AQY of 44.68 % at 420 nm. The photoelectrochemical tests (LSV, I-T, EIS, PL, and TR-PL), ESR, and TRPL were applied to qualitatively demonstrate the function of AgxPdy nano-cocatalyst, and the testing results indicated that the cocatalyst significantly enhances the separation and transfer efficiency of photoinduced electrons, while further lowering the hydrogen evolution reaction energy barrier. Based on that, affecting mechanism was further determined through DFT simulation quantitatively. The prediction results indicated that the unique nanoclusters structure of AgPd3 contribute with the high work function and low d band center position increase the transfer efficiency of the photoinduced charge carriers. This study quantitatively revealed the relationship among compostion, structure and reactivity of the photocatalysts, provided an method to investigate the affecting mechanism of bimetallic hydrogen evolution photocatalysts and contributed to the advancement of renewable energy development.</div></div>\",\"PeriodicalId\":337,\"journal\":{\"name\":\"International Journal of Hydrogen Energy\",\"volume\":\"116 \",\"pages\":\"Pages 378-388\"},\"PeriodicalIF\":8.3000,\"publicationDate\":\"2025-03-13\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"International Journal of Hydrogen Energy\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0360319925012716\",\"RegionNum\":2,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"International Journal of Hydrogen Energy","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0360319925012716","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}

引用次数: 0

摘要

贵金属负载策略是提高CdS基光催化剂在可见光下裂解水析氢反应活性的有效方法。该策略的关键问题是影响机理，而影响机理是由负载金属的组成、种类和结构决定的。本研究制备了AgPd双金属纳米团簇（AgxPdy），并将其加载到雪花状cd表面，通过仪器分析和计算方法对其影响机理进行了定性和定量研究。通过XRD、TEM和XPS对合成样品的组成和结构进行了表征，证实了AgPd双金属纳米团簇合金的成功合成，平均粒径约为3 nm。进一步测试了agxpd3 /CdS在可见光下的析氢性能，制备的AgPd3/CdS的析氢速率为73.93 mmol h−1 g−1，比Pd/CdS提高了28%，比cd提高了381%，在420 nm处的AQY为44.68%。利用光电化学测试（LSV、I-T、EIS、PL和TR-PL）、ESR和TRPL等方法定性地验证了AgxPdy纳米助催化剂的功能，测试结果表明，该助催化剂显著提高了光诱导电子的分离和转移效率，同时进一步降低了析氢反应的能垒。在此基础上，通过DFT仿真进一步定量确定了影响机理。预测结果表明，AgPd3独特的纳米团簇结构、高功函数和低d带中心位置有助于提高光诱导载流子的转移效率。本研究定量揭示了光催化剂的组成、结构和反应性之间的关系，为探讨双金属析氢光催化剂的影响机理提供了一种方法，有助于推动可再生能源的发展。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

查看原文本刊更多论文

A AgPd3/2D-CdS photocatalyst: The function of AgPd3 cocatalyst, and the enhanced photocatalytic hydrogen generation property under visible light

Precious metals loading strategy is an effective method to increase the reactivity of CdS based photocatalysts for hydrogen evolution from water splitting under visible light. The key problem of such strategy is the affecting mechanism, which determined by the composition, species and structure of the loaded metals. In this study, AgPd bimetallic nanoclusters (Ag_xPd_y) were prepared and then loaded onto the surface of snowflake-like CdS and the affecting mechanism was qualitatively and quantatively investigated through both instrumental analysis and computational method. The composition and structure of synthesized samples were examined through XRD, TEM, and XPS, by which the successful synthesis of AgPd bimetallic nanocluster alloys with an average particle size of approximately 3 nm were confirmed. Further, the hydrogen evolution performance of Ag_xPd_y/CdS was tested under visible light and the prepared AgPd₃/CdS achieved a hydrogen evolution rate of 73.93 mmol h⁻¹ g⁻¹, which is a 28 % improvement over Pd/CdS and a 381 % improvement over CdS, with an AQY of 44.68 % at 420 nm. The photoelectrochemical tests (LSV, I-T, EIS, PL, and TR-PL), ESR, and TRPL were applied to qualitatively demonstrate the function of Ag_xPd_y nano-cocatalyst, and the testing results indicated that the cocatalyst significantly enhances the separation and transfer efficiency of photoinduced electrons, while further lowering the hydrogen evolution reaction energy barrier. Based on that, affecting mechanism was further determined through DFT simulation quantitatively. The prediction results indicated that the unique nanoclusters structure of AgPd₃ contribute with the high work function and low d band center position increase the transfer efficiency of the photoinduced charge carriers. This study quantitatively revealed the relationship among compostion, structure and reactivity of the photocatalysts, provided an method to investigate the affecting mechanism of bimetallic hydrogen evolution photocatalysts and contributed to the advancement of renewable energy development.

求助全文

通过发布文献求助，成功后即可免费获取论文全文。去求助

来源期刊

International Journal of Hydrogen Energy 工程技术-环境科学

CiteScore

13.50

自引率

25.00%

发文量

3502

审稿时长

60 days

期刊介绍： The objective of the International Journal of Hydrogen Energy is to facilitate the exchange of new ideas, technological advancements, and research findings in the field of Hydrogen Energy among scientists and engineers worldwide. This journal showcases original research, both analytical and experimental, covering various aspects of Hydrogen Energy. These include production, storage, transmission, utilization, enabling technologies, environmental impact, economic considerations, and global perspectives on hydrogen and its carriers such as NH3, CH4, alcohols, etc. The utilization aspect encompasses various methods such as thermochemical (combustion), photochemical, electrochemical (fuel cells), and nuclear conversion of hydrogen, hydrogen isotopes, and hydrogen carriers into thermal, mechanical, and electrical energies. The applications of these energies can be found in transportation (including aerospace), industrial, commercial, and residential sectors.