C2N-supported single metal ion catalysts for HCOOH dehydrogenation

被引：46

作者：

Zhong, Wenhui ^{[1
]}

Liu, Yuxia ^{[2
]}

Deng, Mingsen ^{[1
]}

Zhang, Yachao ^{[1
]}

Jia, Chuanyi ^{[1
]}

Prezhdo, Oleg V. ^{[3
]}

Yuan, Jianyong ^{[4
]}

Jiang, Jun ^{[5
]}

机构：

[1] Guizhou Educ Univ, Guizhou Prov Key Lab Computat Nanomat Sci, Inst Appl Phys, Guizhou Synerget Innovat Ctr Sci Big Data Adv Mfg, Gaoxin Rd 115, Guiyang 550018, Guizhou, Peoples R China

[2] Qufu Normal Univ, Sch Chem & Chem Engn, Qufu 273165, Peoples R China

[3] Univ Southern Calif, Dept Chem, Los Angeles, CA 90089 USA

[4] East China Univ Sci & Technol, Sch Mat Sci & Engn, Shanghai Key Lab Adv Polymer Mat, Key Lab Ultrafine Mat,Minist Educ, Shanghai 200237, Peoples R China

[5] Univ Sci & Technol China, CAS Key Lab Mech Behav & Design Mat, IChEM Collaborat Innovat Ctr Chem Energy Mat, Hefei Natl Lab Phys Sci Microscale,Sch Chem & Mat, Hefei 230026, Anhui, Peoples R China

来源：

JOURNAL OF MATERIALS CHEMISTRY A | 2018年 / 6卷 / 24期

基金：

中国国家自然科学基金;

关键词：

REDUCED GRAPHENE OXIDE; FORMIC-ACID OXIDATION; N-DOPED CARBON; HYDROGEN-PRODUCTION; FACILE SYNTHESIS; OXYGEN; CO; NANOPARTICLES; MECHANISM; DECOMPOSITION;

D O I：

10.1039/c8ta02299b

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：

High catalytic performance of a single-atom transition metal ion (TMx+) anchored on the two-dimensional (2D) C2N lattice is predicted for HCOOH dehydrogenation. Considering the Co2+, Cu2+ and Ni2+ non-noble metal ions supported by C2N, we use density functional theory to demonstrate dehydrogenation energy barriers as low as those for pure Pt and Pd catalysts. The high catalytic performance is ascribed to the reaction occurring through a dual-active center composed of TMx+ and a nearby N atom of C2N. Specifically, C2N-Co2+ in the low spin state (S = 1/2) greatly promotes HCOOH dehydrogenation by decreasing the barrier of the rate-determining step to only 0.30 eV, mainly due to the strong ability of TMx+ to extract charges from HCOOH and C2N. The obtained mechanistic insights help the rational design of single-atom based transition metal ion catalysts supported by 2D materials.

引用

页码：11105 / 11112

页数：8

共 50 条

[31] Activities of γ-Al2O3-supported metal oxide catalysts in propane oxidative dehydrogenation
Al-Zahrani, SM
Jibril, BY
Abasaeed, AF
CATALYSIS LETTERS, 2003, 85 (1-2) : 57 - 67
[32] Oxidative dehydrogenation of isobutane to isobutylene over supported transition metal oxide catalysts
Hoang, M
Mathews, JF
Pratt, KC
REACTION KINETICS AND CATALYSIS LETTERS, 1997, 61 (01): : 21 - 26
[33] EFFECT OF GAMMA-RADIATION ON SUPPORTED METAL-CATALYSTS OF CYCLOHEXANE DEHYDROGENATION
GYORGY, I
SZAUER, G
FOLDIAK, G
PAAL, Z
ZEITSCHRIFT FUR PHYSIKALISCHE CHEMIE-WIESBADEN, 1982, 132 (02): : 241 - 249
[34] Oxidative Dehydrogenation of Light Alkanes on Supported Molten Alkali Metal Chloride Catalysts
Chinthala Praveen Kumar
Stefan Gaab
Thomas E. Müller
Johannes A. Lercher
Topics in Catalysis, 2008, 50 : 156 - 167
[35] Supported chromium oxide catalysts using metal carboxylate complexes:: dehydrogenation of propane
Gorriz, OF
Cadús, LE
APPLIED CATALYSIS A-GENERAL, 1999, 180 (1-2) : 247 - 260
[36] Catalytic dehydrogenation for hydrogen production controlled by metal-supported heterogeneous catalysts
Choi, Yuyeol
Wu, Xinkai
Lee, Ji-Woong
Na, Kyungsu
CATALYSIS SCIENCE & TECHNOLOGY, 2024, 14 (20) : 5784 - 5810
[37] SUPPORTED SNO2 CATALYSTS FOR THE OXIDATIVE DEHYDROGENATION OF ETHYLBENZENE
TAGAWA, T
KATAOKA, S
HATTORI, T
MURAKAMI, Y
APPLIED CATALYSIS, 1982, 4 (01): : 1 - 4
[38] Supported vanadia catalysts for dehydrogenation of ethylbenzene with CO2
Li, XH
Li, WY
Xie, KC
CATALYSIS LETTERS, 2005, 105 (3-4) : 223 - 227
[39] Coupling of N2O decomposition and ethylbenzene dehydrogenation over γ-Al2O3-supported transition metal oxide catalysts
Kustrowski, P
Zbroja, M
Dziembaj, R
Papp, H
CATALYSIS LETTERS, 2002, 80 (1-2) : 1 - 6
[40] Coupling of N2O Decomposition and Ethylbenzene Dehydrogenation over γ-Al2O3-Supported Transition Metal Oxide Catalysts
Piotr Kuśtrowski
Małgorzata Zbroja
Roman Dziembaj
Helmut Papp
Catalysis Letters, 2002, 80 : 1 - 6

← 1 2 3 4 5 →