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构建C、O共掺杂氮化硼与钯铜合金纳米晶体之间的吸附和光催化界面以实现CO向CO的有效转化。

Construction adsorption and photocatalytic interfaces between C, O co-doped BN and Pd-Cu alloy nanocrystals for effective conversion of CO to CO.

作者信息

Yang Yang, Shen Zhangfeng, Yang Hanwu, Zou Xuhui, Meng Yuxiao, Jiang Lingchang, Liu Yanan, Xia Qineng, Cao Yongyong, Li Xi, Gao Jing, Wang Yangang

机构信息

College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310032, China; College of Biological Chemical Science and Engineering, Jiaxing University, Jiaxing 314001, China.

College of Biological Chemical Science and Engineering, Jiaxing University, Jiaxing 314001, China.

出版信息

J Colloid Interface Sci. 2023 Jun 15;640:949-960. doi: 10.1016/j.jcis.2023.02.146. Epub 2023 Mar 2.

Abstract

Photocatalytic reduction of carbon dioxide (CO) into fuels is an auspicious route to alleviate the energy and environmental crisis brought by the continuous depletion of fossil fuels. The CO adsorption state on the surface of photocatalytic materials plays a significant role in its efficient conversion. The limited CO adsorption capacity of conventional semiconductor materials inhibit their photocatalytic performances. In this work, a bifunctional material for CO capture and photocatalytic reduction was fabricated by introducing palladium (Pd)-copper (Cu) alloy nanocrystals onto the surface of carbon, oxygen co-doped boron nitride (BN). The elemental doped BN with abundant ultra-micropores had high CO capture ability, and CO was adsorbed in the form of bicarbonate on its surface with the presence of water vapor. The Pd/Cu molar ratio had great impact on the grain size of Pd-Cu alloy and their distribution on BN. The CO molecules tended to be converted to carbon monoxide (CO) at interfaces of BN and Pd-Cu alloys due to their bidirectional interactions to the adsorbed intermediate species while methane (CH) evolution might occur on the surface of Pd-Cu alloys. Owing to the uniform distribution of smaller Pd-Cu nanocrystals on BN, more effective interfaces were created in the PdCu/BN sample and it gave a CO production rate of 7.74 μmolgh under simulated solar light irradiation, higher than the other PdCu/BN composites. This work can pave a new way for constructing effective bifunctional photo-catalysts with high selectivity to convert CO to CO.

摘要

光催化将二氧化碳(CO₂)还原为燃料是缓解化石燃料持续枯竭所带来的能源和环境危机的一条可行途径。光催化材料表面的CO₂吸附状态对其高效转化起着重要作用。传统半导体材料有限的CO₂吸附能力限制了它们的光催化性能。在这项工作中,通过将钯(Pd)-铜(Cu)合金纳米晶体引入碳、氧共掺杂的氮化硼(BN)表面,制备了一种用于CO₂捕获和光催化还原的双功能材料。具有丰富超微孔的元素掺杂BN具有高CO₂捕获能力,在有水蒸气存在的情况下,CO₂以碳酸氢盐的形式吸附在其表面。Pd/Cu摩尔比对Pd-Cu合金的晶粒尺寸及其在BN上的分布有很大影响。由于CO分子与吸附的中间物种的双向相互作用,它们倾向于在BN和Pd-Cu合金的界面处转化为一氧化碳(CO),而甲烷(CH₄)的生成可能发生在Pd-Cu合金表面。由于较小的Pd-Cu纳米晶体在BN上均匀分布,PdCu/BN样品中形成了更有效的界面,在模拟太阳光照射下其CO生成速率为7.74 μmol·g⁻¹·h⁻¹,高于其他PdCu/BN复合材料。这项工作可为构建具有高选择性将CO₂转化为CO的有效双功能光催化剂开辟一条新途径。

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