电子结构不对称碳介导的Pd电荷重分布促进乙醇氧化反应

引用本文: 周鑫灿, 王雪瑶, 陈小康, 兰笛, 高宇庭, 王晓霞, 李道浩, 张树超, 张立杰, 吴广磊. 电子结构不对称碳介导的Pd电荷重分布促进乙醇氧化反应[J]. 物理化学学报, 2026, 42(7): 100287. doi: 10.1016/j.actphy.2026.100287 shu

Citation: Xincan Zhou, Xueyao Wang, Xiaokang Chen, Di Lan, Yuting Gao, Xiaoxia Wang, Daohao Li, Shuchao Zhang, Lijie Zhang, Guanglei Wu. Charge redistribution on Pd mediated by electronically asymmetric carbon for boosting ethanol oxidation[J]. Acta Physico-Chimica Sinica, 2026, 42(7): 100287. doi: 10.1016/j.actphy.2026.100287 shu

电子结构不对称碳介导的Pd电荷重分布促进乙醇氧化反应

周鑫灿 ^1,2, ,
王雪瑶 ^1,3, ,
陈小康 ^1,4, ,
兰笛 ^2, ,
高宇庭 ^5, ,
王晓霞 ^1, ,
李道浩 ^1, ,
张树超 ^{1,6,
,} ,
张立杰 ^{1,
,} ,
吴广磊 ^{1,
,}

1.
青岛大学材料科学与工程学院, 生物纤维与生态纺织国家重点实验室, 山东青岛 266071;
2.
湖北汽车工业学院汽车材料学院, 湖北十堰 442002;
3.
山东大学环境科学与工程学院, 山东青岛 266237;
4.
山东大学化学与化工学院前沿化学研究院, 山东青岛 266237;
5.
山东省科学技术情报研究院, 山东济南 250101;
6.
青岛大学附属医院输血科, 山东青岛 266003

通讯作者: 张树超,E-mail:zhangshuchao@qdu.edu.cn; 张立杰,E-mail:lijiezh@qdu.edu.cn; 吴广磊,E-mail:wuguanglei@qdu.edu.cn/wuguanglei@mail.xjtu.edu.cn

基金项目:
本工作得到了国家自然科学基金8257028和52377026)、泰山学者计划(tsqn202211124和tsqn202103057)、山东省自然科学基金(ZR2022QB023)以及山东省高等学校青创人才引育计划(海洋多糖纤维基能源材料研究与创新团队)的资助。

摘要: 作为一类具有应用前景的乙醇氧化反应(EOR)催化剂，Pd基材料仍然本征受限于表面电子结构在乙醇吸附与CH₃CO中间体脱附之间的权衡关系。本文合成了负载于N/S共掺杂碳上的Pd催化剂(Pd@SNC)，其中掺杂的S和N原子能够向Pd转移适量电子，从而赋予Pd更为适宜的电子结构。此外，d带中心的适度负移表明，该适宜的Pd电子结构不仅能够增强对乙醇和OH^-的吸附，还能够促进中间体(CH₃CO*)的脱附，从而有利于反应动力学。结果表明，Pd@SNC表现出最高的EOR催化活性，其质量活性达到945.49 mA mgPd^-1，明显优于Pd@NC和Pd@C。理论计算结果进一步表明，由于共掺杂N和S原子对Pd电子结构进行了有效调控，Pd@SNC在EOR过程中脱氢步骤表现出最低的反应能垒。

关键词:

English

Charge redistribution on Pd mediated by electronically asymmetric carbon for boosting ethanol oxidation

1.
State Key Laboratory of Bio-fibers and Eco-textiles, College of Materials Science and Engineering, Qingdao University, Qingdao 266237, Shandong Province, China;
2.
School of Automotive Materials, Hubei University of Automotive Technology, Shiyan 442002, Hubei Province, China;
3.
School of Environmental Science and Engineering, Shandong University, Qingdao 266237, Shandong Province, China;
4.
Institute of Frontier Chemistry, School of Chemistry and Chemical Engineering, Shandong University, Qingdao 266237, Shandong Province, China;
5.
Shandong Institute of Scientific and Technical Information, Jinan 250101, Shandong Province, China;
6.
Department of Blood Transfusion, The Affiliated Hospital of Qingdao University, Qingdao University, Qingdao 266003, Shandong Province, China

Corresponding author: Shuchao Zhang, ; Lijie Zhang, ; Guanglei Wu,

Received Date: 19 December 2025
Accepted Date: 12 March 2026
Revised Date: 12 March 2026

Abstract: Pd-based materials as the promising catalysts for ethanol oxidation reaction (EOR) are still intrinsically limited by the surface electronic-structure trade-off between ethanol adsorption and CH₃CO intermediate desorption. Herein, the Pd supported on N/S co-doped carbon (Pd@SNC) catalyst is synthesized, in which the doped S and N atoms could transfer moderate amounts electron to Pd, leading to opportune electron structure of Pd. Moreover, the moderate negative shift of d-band center demonstrate that the opportune Pd electron structure can strengthen adsorption of ethanol/OH^- and promote the desorption of intermediate (CH₃CO*), which may facilitate the kinetics. As a result, Pd@SNC exhibiting the highest catalytic activity for EOR (945.49 mA mg_Pd^-1), surpassing to that of Pd@NC and Pd@C. Due to the fact that the electronic structure of Pd is properly regulated by co-doped N and S atoms, as shown by the theoretical calculation results, Pd@SNC exhibits the lowest reaction energy barrier of the dehydrogenation during the process of EOR.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

电子结构不对称碳介导的Pd电荷重分布促进乙醇氧化反应

通讯作者: 张树超,E-mail:zhangshuchao@qdu.edu.cn; 张立杰,E-mail:lijiezh@qdu.edu.cn; 吴广磊,E-mail:wuguanglei@qdu.edu.cn/wuguanglei@mail.xjtu.edu.cn

English

Charge redistribution on Pd mediated by electronically asymmetric carbon for boosting ethanol oxidation

Corresponding author: Shuchao Zhang, ; Lijie Zhang, ; Guanglei Wu,

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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中国化学会秘书处

电子结构不对称碳介导的Pd电荷重分布促进乙醇氧化反应

通讯作者: 张树超,E-mail:zhangshuchao@qdu.edu.cn; 张立杰,E-mail:lijiezh@qdu.edu.cn; 吴广磊,E-mail:wuguanglei@qdu.edu.cn/wuguanglei@mail.xjtu.edu.cn

English

Charge redistribution on Pd mediated by electronically asymmetric carbon for boosting ethanol oxidation

Corresponding author: Shuchao Zhang, ; Lijie Zhang, ; Guanglei Wu,

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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