High-Loading Single-Atom Ru Catalysts Anchored on N-Doped Graphdiyne/?-Graphyne Quantum Dots for Selective Hydrodehalogenation and Hydrodearomatization

被引：7
|
作者：
Zhang, Chao [1 ,2 ,3 ,4 ,5 ]
Li, Yingqiang [1 ,2 ,3 ]
Xie, Yue [1 ,2 ,3 ]
Yu, Zhanjiang [1 ,2 ,3 ]
Wan, Xin [1 ,2 ,3 ]
Wang, Xinzhi [1 ,2 ,3 ]
He, Jiaan [1 ,2 ,3 ]
Li, Junlang [1 ,2 ,3 ]
Chen, Zhenguo [1 ,2 ,3 ]
Li, Xiaoyong [1 ,2 ,3 ]
Yi, Xiaohui [1 ,2 ,3 ]
Wang, Zhaoli [4 ,6 ]
Ying, Guang-Guo [1 ,2 ,3 ]
Dionysiou, Dionysios D. [5 ]
Huang, Mingzhi [1 ,2 ,3 ]
机构：
[1] South China Normal Univ, SCNU NANAN Green & Low Carbon Innovat Ctr, Guangdong Prov Engn Res Ctr Intelligent Low Carbo, Sch Environm, Guangzhou 510006, Peoples R China
[2] South China Normal Univ, Sch Environm, Guangdong Prov Key Lab Chem Pollut & Environm Saf, Guangzhou 510006, Peoples R China
[3] South China Normal Univ, Sch Environm, MOE Key Lab Theoret Chem Environm, Guangzhou 510006, Peoples R China
[4] South China Univ Technol, Sch Civil Engn & Transportat, State Key Lab Subtrop Bldg & Urban Sci, State Key Lab Subtrop Bldg Sci, Guangzhou 510641, Peoples R China
[5] Univ Cincinnati, Dept Chem & Environm Engn ChEE, Environm Engn & Sci Program, Cincinnati, OH 45221 USA
[6] Pazhou Lab, Guangzhou 510335, Peoples R China
来源：
ACS CATALYSIS | 2023年 / 13卷 / 18期
基金：
中国国家自然科学基金;
关键词：
water remediation; selective hydrodehalogenation and hydrodearomatization; single-atom catalysts; graphdiyne; quantum dots; NANOPARTICLES; NANOCLUSTERS; NANOTUBES; RUTHENIUM; PLATINUM; ROUTE;
D O I：
10.1021/acscatal.3c01390
中图分类号：
O64 [物理化学（理论化学）、化学物理学];
学科分类号：
070304 ; 081704 ;
摘要：
Selective hydrodehalogenation and hydrodearomatization of toxic chlorophenols into value-added chemicals represents a grand challenge for their efficient reutilization. For this purpose, single-atom catalysts (SACs) could be a strategy with relatively high catalytic selectivity and atom utilization but suffer from the catalytic limitation caused by low metal loading densities. Graphdiyne and ?-graphyne are considered promising substrates of SACs with excellent catalytic properties. Additionally, their quantum dots with nanometer size are expected to supply numerous surface anchoring sites and large atom spacing to confine metal cations to synthesize high-loading SACs. Here we report a synthesis approach for high-loading Ru SACs anchored on graphdiyne/?-graphyne quantum dots (GDQD-Ru/GNQD-Ru), which exhibit remarkably higher turnover frequency (TOF) and selectivity (>99%) of hydrodehalogenation and hydrodearomatization of chlorophenols than graphdiyne/?-graphyne nanosheet-based Ru SACs and nanoparticles. There is no significant selectivity decrease in chlorophenol transformation by GDQD-Ru/GNQD-Ru observed in 5 catalyst reuse cycles. GDQD-Ru/GNQD-Ru contribute to nearly exclusive hydrodehalogenation and hydrodearomatization without altering any other bonds in chlorophenols. Experimental results and theoretical calculations reveal that GDQD-Ru is more prone to lower energies of rate-limiting steps in H-2-driven chlorophenol transformation than GNQD-Ru. The results confirm that graphdiyne/?-graphyne quantum dots play crucial roles in facilitating the metal atom loading of SACs. Ru loadings are 27.6 and 16.0 wt % in GDQD-Ru/GNQD-Ru, approximately 7-fold and 4-fold higher than reported Ru SACs, respectively. This study provides mechanistic insights toward the roles of high-loading Ru SACs on sp- and sp(2)-hybridized carbonaceous substrates in selective hydrodehalogenation and hydrodearomatization.
引用
收藏
页码：12425 / 12435
页数：11
相关论文
共 50 条
  • [21] Non-metal iodine single-atom catalysts anchored on N-doped graphene for high-performance lithium-sulfur battery
    Li, Xue
    Yu, Jiaqi
    Li, Wenzhuo
    Liao, Yalan
    Li, Meng
    Zhao, Bing
    Liu, Xiaoyu
    Huang, Shoushuang
    Xia, Shuixin
    Zhang, Jiujun
    Jiang, Yong
    CHEMICAL ENGINEERING JOURNAL, 2025, 505
  • [22] A Quantum Signature for Catalytic Activity in N-doped, Single-Atom Fe Electrocatalysts
    Zhong, Hong
    Barr, Jordan A.
    Beckman, Scott P.
    CATALYSIS LETTERS, 2024, 154 (06) : 2590 - 2596
  • [23] A Quantum Signature for Catalytic Activity in N-doped, Single-Atom Fe Electrocatalysts
    Hong Zhong
    Jordan A. Barr
    Scott P. Beckman
    Catalysis Letters, 2024, 154 : 2590 - 2596
  • [24] Iron Single-Atom Anchored on N-Doped Carbon Nanozymes for Chlorpyrifos Detection and Antibacterial Applications
    Ren, Enxiang
    Zhang, Xing
    Lu, Guo-Ping
    Sohail, Muhammad
    Hu, Jun
    Chen, Zhong
    Fan, Daidi
    Lin, Yamei
    ACS APPLIED NANO MATERIALS, 2023, 6 (16) : 15038 - 15047
  • [25] High-loading single-atom tungsten anchored on graphitic carbon nitride (melon) for efficient oxidation of emerging contaminants
    Gu, Yan
    Xu, Tiefeng
    Chen, Xiufang
    Chen, Wenxing
    Lu, Wangyang
    CHEMICAL ENGINEERING JOURNAL, 2022, 427
  • [26] High-loading As single-atom catalysts harvested from wastewater towards efficient and sustainable oxygen reduction
    Luo, Yangjun
    Wang, Yanwei
    Zhang, Huijuan
    Wang, Youyuan
    Wan, Jin
    Feng, Chuanzhen
    Liu, Lingmei
    Guo, Zaiping
    Li, Jian
    Wang, Yu
    ENERGY & ENVIRONMENTAL SCIENCE, 2024, 17 (01) : 123 - 133
  • [27] Design of Efficient Oxygen Reduction Reaction Catalysts with Single Transition Metal Atom on N-Doped Graphdiyne
    Zou, Min
    Yang, Jing
    Yue, Xiaolong
    Yuan, Yanan
    Che, Zhongmei
    Li, Mei
    Li, Bo
    Cui, Jiaxi
    Hu, Wei
    Wang, Shuai
    Jiang, Jun
    Jia, Chuanyi
    JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 2023, 14 (43): : 9624 - 9632
  • [28] Ball-milling Synthesis of Single-atom Cu Anchored on N-Doped Carbon for Mimicking Peroxidase
    Henan Xu
    Lingling Zhang
    Huilin Wang
    Shaopeng Zhang
    Wei Li
    Xiao Wang
    Shuyan Song
    Daguang Wang
    Zhan Shi
    Chemical Research in Chinese Universities, 2023, 39 : 948 - 953
  • [29] The Key Role of Competition between Orbital and Electrostatic Interactions in the Adsorption on Transition Metal Single-Atom Catalysts Anchored by N-doped Graphene
    Zhang, Nan-Nan
    Li, Jun
    Xiao, Hai
    CHEMCATCHEM, 2022, 14 (16)
  • [30] Single-Atom Iron Nanozymes Anchored on Graphitic N-Doped Carbon for Visual Alkaline Phosphatase Detection
    Wu, Shumin
    Tao, Chenyu
    Xu, Peng
    Liu, Wendong
    Xia, Mingyuan
    Jiang, Yuanyuan
    Lu, Yizhong
    ACS APPLIED NANO MATERIALS, 2025,
12345