Highly efficient and durable aqueous electrocatalytic reduction of CO2 to HCOOH with a novel bismuth–MOF: experimental and DFT studies,Journal of Materials Chemistry A

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Highly efficient and durable aqueous electrocatalytic reduction of CO2 to HCOOH with a novel bismuth–MOF: experimental and DFT studies
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2020-04-24 , DOI: 10.1039/d0ta00384k
Xurui Zhang _{1,

2,

3,

4,

5} , Yanxing Zhang _{5,

6,

7,

8,

9} , Qingqing Li _{1,

2,

3,

4,

5} , Xiaodong Zhou _{9,

10,

11,

12} , Qingyu Li _{5,

13,

14,

15,

16} , Jin Yi _{1,

2,

3,

4,

5} , Yuyu Liu _{1,

2,

3,

4,

5} , Jiujun Zhang _{1,

2,

3,

4,

5}

Affiliation

Institute for Sustainable Energy
College of Sciences
Shanghai University
Shanghai 200444
China
School of Physics
Henan Normal University
Xinxiang
Department of Chemical Engineering
University of Louisiana at Lafayette
Lafayette
USA
Guangxi Key Laboratory of Low Carbon Energy Materials
School of Chemical and Pharmaceutical Science
Guangxi Normal University
Guilin

Electrochemical reduction of carbon dioxide (ERCO₂) to low-carbon fuel and useful chemicals, which can simultaneously store renewable energy and recover CO₂ in a green manner, has proven to be a viable energy storage and conversion strategy. However, there is always a technical bottleneck in preparation of highly active, selective and stable catalysts. In this work, we hydrothermally synthesized a new type of bismuth-based organic framework (Bi–MOF) and carefully investigated it as the catalyst for ERCO₂. All the samples exhibited excellent performance and the optimized one (i.e. Bi-BTC-D) achieved a high formate Faraday efficiency (FE) up to 95.5% at −0.86 V_RHE and a current density of −11.2 mA cm⁻². Moreover, the FE has been maintained over 90.0% after 12 hours of continuous electrolysis without significant reduction. The measurement results demonstrated that the excellent performance can be attributed to the special structure of Bi-BTC-D. DFT calculations show that the Bi site of Bi-BTC-D is highly efficient for formate production with very low overpotentials. The great potential of using a Bi–MOF as a highly stable, molecularly tunable catalytic material for ERCO₂ is confirmed.

中文翻译：

新型铋-MOF高效持久地水催化将CO2还原为HCOOH：实验和DFT研究

将二氧化碳（ERCO ₂）电化学还原为低碳燃料和有用的化学物质可同时存储可再生能源并以绿色方式回收CO ₂，已被证明是可行的能量存储和转换策略。但是，制备高活性，选择性和稳定的催化剂始终存在技术瓶颈。在这项工作中，我们水热合成了一种新型的铋基有机骨架（Bi-MOF），并对其进行了认真的研究，以作为ERCO ₂的催化剂。所有样品均表现出出色的性能，经过优化的样品（即Bi-BTC-D）在-0.86 V _RHE和电流密度为-11.2 mA cm时达到了高达95.5％的高甲酸根法拉第效率（FE）。⁻²。此外，在连续电解12小时后，FE保持在90.0％以上，而没有明显的还原。测量结果表明，优异的性能可以归因于Bi-BTC-D的特殊结构。DFT计算表明，Bi-BTC-D的Bi部位对于甲酸生产非常有效，且超电势非常低。事实证明，将Bi-MOF用作ERCO₂的高度稳定的分子可调催化材料具有巨大潜力。

更新日期：2020-04-24

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