三维交联碳纳米网催化剂在空气条件下加速过氧化氢的高效酸性电合成

IF 7.3 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Huiyao Qi, Lilong Zhang, Chang Zhang, Hongshang Hu, Siqi Zhao, Lipiao Bao, Muneerah Alomar, Jian Zhang* and Xing Lu*, 
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引用次数: 0

摘要

通过双电子氧还原反应(2e - ORR)电合成过氧化氢(H2O2)为目前能源密集型的蒽醌工艺提供了一种绿色和可持续的替代方案。然而,在酸性和空气条件下开发廉价高效的电催化剂仍然是一个挑战。本文以天然多孔交联水葫芦骨架为原料,构建了三维氮掺杂碳纳米网(3D-N-CNW)电催化剂。3D-N-CNW具有1464 m2 g-1的超高比表面积,具有相互连接的分层多孔结构和丰富的碳缺陷,具有优异的2e - ORR活性,具有高起始电位(0.64 V)和H2O2选择性(~ 93%),是酸性介质中性能最好的碳基催化剂。令人印象深刻的是,利用3D-N-CNW的液流电池在空气自呼吸条件下实现了4289 mg L-1 h-1的超高H2O2产率,实现了对代表性有机污染物的超快速降解。理论计算和控制实验表明,三维交联网络有利于物质传输,创造了丰富的O2微环境,促进了2e - ORR高效生成H2O2。这项工作为从天然生物质材料中构建先进的碳基电催化剂提供了一种低成本、易于扩展和方便的途径;其他可再生能源领域也有望实现这一目标。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Highly Efficient Acidic Electrosynthesis of Hydrogen Peroxide in Air-Fed Conditions Accelerated by a Three-Dimensional Cross-Linked Carbon Nanoweb Catalyst

Highly Efficient Acidic Electrosynthesis of Hydrogen Peroxide in Air-Fed Conditions Accelerated by a Three-Dimensional Cross-Linked Carbon Nanoweb Catalyst

Electrosynthesis of hydrogen peroxide (H2O2) via a two-electron oxygen reduction reaction (2e ORR) provides a green and sustainable alternative to the current energy-intensive anthraquinone process. However, the development of inexpensive and efficient electrocatalysts under acidic and air-fed conditions remains a challenge. Herein, we constructed a three-dimensional nitrogen-doped carbon nanoweb (3D-N-CNW) electrocatalyst by using a naturally porous cross-linked skeleton of water hyacinth as a raw material. The 3D-N-CNW shows an ultrahigh specific surface area of 1464 m2 g–1 with interconnected hierarchical porous architecture, and abundant carbon defects, resulting in excellent 2e ORR activity with high onset potential (0.64 V) and H2O2 selectivity (∼93%), which is the best-performing carbon-based catalyst reported in acidic media. Impressively, the flow cell utilizing 3D-N-CNW achieves an exceptionally high H2O2 yield of 4289 mg L–1 h–1 under air self-breathing conditions, enabling ultrafast degradation of representative organic pollutants. Theoretical calculations and control experiments reveal that the 3D cross-linked network facilitates mass transport and creates an enriched O2 microenvironment to promote the 2e ORR to highly efficient H2O2 production. This work provides a low-cost, readily scalable, and convenient route for the construction of advanced carbon-based electrocatalysts from natural biomass materials; it can also be expected in other renewable areas.

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来源期刊
ACS Sustainable Chemistry & Engineering
ACS Sustainable Chemistry & Engineering CHEMISTRY, MULTIDISCIPLINARY-ENGINEERING, CHEMICAL
CiteScore
13.80
自引率
4.80%
发文量
1470
审稿时长
1.7 months
期刊介绍: ACS Sustainable Chemistry & Engineering is a prestigious weekly peer-reviewed scientific journal published by the American Chemical Society. Dedicated to advancing the principles of green chemistry and green engineering, it covers a wide array of research topics including green chemistry, green engineering, biomass, alternative energy, and life cycle assessment. The journal welcomes submissions in various formats, including Letters, Articles, Features, and Perspectives (Reviews), that address the challenges of sustainability in the chemical enterprise and contribute to the advancement of sustainable practices. Join us in shaping the future of sustainable chemistry and engineering.
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