Species mass transfer governs the selectivity of gas diffusion electrodes toward H2O2 electrosynthesis

电合成 扩散 传质 选择性 电极 化学 化学物理 纳米技术 材料科学 电化学 催化作用 物理 色谱法 物理化学 热力学 生物化学
作者
Lele Cui,Бин Чэн,Dongxu Chen,Chen He,Yi Liu,Hongyi Zhang,Jian Qiu,Le Liu,Wenheng Jing,Zhenghua Zhang
出处
期刊:Nature Communications [Springer Nature]
卷期号:15 (1)
标识
DOI:10.1038/s41467-024-55091-3
摘要

The meticulous design of advanced electrocatalysts and their integration into gas diffusion electrode (GDE) architectures is emerging as a prominent research paradigm in the H2O2 electrosynthesis community. However, it remains perplexing that electrocatalysts and assembled GDE frequently exhibit substantial discrepancies in H2O2 selectivity during bulk electrolysis. Here, we elucidate the pivotal role of mass transfer behavior of key species (including reactants and products) beyond the intrinsic properties of the electrocatalyst in dictating electrode-scale H2O2 selectivity. This tendency becomes more pronounced in high reaction rate (current density) regimes where transport limitations are intensified. By utilizing diffusion-related parameters (DRP) of GDEs (i.e., wettability and catalyst layer thickness) as probe factors, we employ both short- and long-term electrolysis in conjunction with in-situ electrochemical reflection-absorption imaging and theoretical calculations to thoroughly investigate the impact of DRP and DRP-controlled local microenvironments on O2 and H2O2 mass transfer. The mechanistic origins of diffusion-dependent conversion selectivity at the electrode scale are unveiled accordingly. The fundamental insights gained from this study underscore the necessity of architectural innovations for mainstream hydrophobic GDEs that can synchronously optimize mass transfer of reactants and products, paving the way for next-generation GDEs in gas-consuming electroreduction scenarios. Electrocatalysts and assembled gas diffusion electrodes frequently exhibit discrepancies in selectivity during H2O2 electrosynthesis. Here, the authors report the pivotal role of key species transport beyond the intrinsic properties of electrocatalysts in dictating electrode-scale H2O2 selectivity.
最长约 10秒,即可获得该文献文件

科研通智能强力驱动
Strongly Powered by AbleSci AI
更新
大幅提高文件上传限制,最高150M (2024-4-1)

科研通是完全免费的文献互助平台,具备全网最快的应助速度,最高的求助完成率。 对每一个文献求助,科研通都将尽心尽力,给求助人一个满意的交代。
实时播报
当当完成签到,获得积分10
刚刚
刚刚
SUE发布了新的文献求助10
1秒前
alex发布了新的文献求助10
1秒前
1秒前
Jozee完成签到,获得积分10
1秒前
2秒前
春锅锅完成签到,获得积分10
3秒前
喜悦的月光完成签到,获得积分10
3秒前
3秒前
科研通AI2S应助hh0采纳,获得10
4秒前
4秒前
CipherSage应助谷粱靖柔采纳,获得30
5秒前
5秒前
思源应助Yeah采纳,获得10
6秒前
6秒前
高兴微笑完成签到,获得积分10
6秒前
1234645678发布了新的文献求助10
6秒前
6秒前
7秒前
7秒前
全球发布了新的文献求助10
7秒前
科研通AI2S应助hhh采纳,获得10
8秒前
科研通AI2S应助咸鱼一号采纳,获得10
8秒前
打打应助xzy998采纳,获得10
9秒前
9秒前
华仔应助小蜗牛采纳,获得10
9秒前
李小宇完成签到,获得积分10
9秒前
春衫发布了新的文献求助10
10秒前
大模型应助dev-evo采纳,获得10
10秒前
sun发布了新的文献求助30
10秒前
cdy完成签到 ,获得积分10
11秒前
浩西发布了新的文献求助10
11秒前
11秒前
上官若男应助大力日记本采纳,获得10
11秒前
Orange应助笨笨行云采纳,获得10
12秒前
深情安青应助小小威廉采纳,获得10
13秒前
Jason完成签到,获得积分10
14秒前
鱼雷发布了新的文献求助10
14秒前
科目三应助李小宇采纳,获得10
14秒前
高分求助中
The late Devonian Standard Conodont Zonation 2000
The Lali Section: An Excellent Reference Section for Upper - Devonian in South China 1500
Nickel superalloy market size, share, growth, trends, and forecast 2023-2030 1000
Smart but Scattered: The Revolutionary Executive Skills Approach to Helping Kids Reach Their Potential (第二版) 1000
Mantiden: Faszinierende Lauerjäger Faszinierende Lauerjäger 800
PraxisRatgeber: Mantiden: Faszinierende Lauerjäger 800
A new species of Coccus (Homoptera: Coccoidea) from Malawi 500
热门求助领域 (近24小时)
化学 医学 生物 材料科学 工程类 有机化学 生物化学 物理 内科学 纳米技术 计算机科学 化学工程 复合材料 基因 遗传学 催化作用 物理化学 免疫学 量子力学 细胞生物学
热门帖子
关注 科研通微信公众号,转发送积分 3245464
求助须知:如何正确求助?哪些是违规求助? 2889085
关于积分的说明 8256869
捐赠科研通 2557437
什么是DOI,文献DOI怎么找? 1386114
科研通“疑难数据库(出版商)”最低求助积分说明 650285
邀请新用户注册赠送积分活动 626541