On the Mechanism Underlying the Direct Conversion of Methane to Methanol by Copper Hosted in Zeolites; Braiding Cu K-Edge XANES and Reactivity Studies

被引：91

作者：

Newton, Mark A. ^{[1
]}

Knorpp, Amy J. ^{[1
]}

Pinar, Ana B. ^{[1
]}

Sushkevich, Vitaly L. ^{[2
]}

Palagin, Dennis ^{[2
]}

van Bokhoven, Jeroen A. ^{[1
,2
]}

机构：

[1] Swiss Fed Inst Technol, Inst Chem & Bioengn, Dept Chem & Appl Biosci, Vladimir Prelog Weg 1-5-10, CH-8093 Zurich, Switzerland

[2] Paul Scherrer Inst, Lab Catalysis & Sustainable Chem, CH-5232 Villigen, Switzerland

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2018年 / 140卷 / 32期

关键词：

ACTIVE-SITE; CATALYTIC CONVERSION; OXIDATION; MORDENITE; ACTIVATION; CLUSTERS; CU-ZSM-5; MONOOXYGENASE; STABILITY; CU-SSZ-13;

D O I：

10.1021/jacs.8b05139

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The application and quantification of in situ copper K-edge X-ray absorption near-edge structure (XANES), when linked to independently made reactor based studies of methanol production, result in a majority relation between the production of Cu-I and methanol from methane that complies with the expectations of a two-electron mechanism founded upon Cu-II/Cu-I redox couples.

引用

页码：10090 / 10093

页数：4

共 46 条

[1] Catalytic conversion of methane to methanol over Cu-mordenite [J].

Alayon, Evalyn Mae ;

Nachtegaal, Maarten ;

Ranocchiari, Marco ;

van Bokhoven, Jeroen A. .

CHEMICAL COMMUNICATIONS, 2012, 48 (03) :404-406

[2] Bis(μ-oxo) versus mono(μ-oxo)dicopper cores in a zeolite for converting methane to methanol: an in situ XAS and DFT investigation [J].

Alayon, Evalyn Mae C. ;

Nachtegaal, Maarten ;

Bodi, Andras ;

Ranocchiari, Marco ;

van Bokhoven, Jeroen A. .

PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2015, 17 (12) :7681-7693

[3] Reaction Conditions of Methane-to-Methanol Conversion Affect the Structure of Active Copper Sites [J].

Alayon, Evalyn Mae C. ;

Nachtegaal, Maarten ;

Bodi, Andras ;

van Bokhoven, Jeroen A. .

ACS CATALYSIS, 2014, 4 (01) :16-22

[4] Determination of the electronic and geometric structure of Cu sites during methane conversion over Cu-MOR with X-ray absorption spectroscopy [J].

Alayon, Evalyn Mae C. ;

Nachtegaal, Maarten ;

Kleymenov, Evgeny ;

van Bokhoven, Jeroen A. .

MICROPOROUS AND MESOPOROUS MATERIALS, 2013, 166 :131-136

[5]

[Anonymous], 2016, XRAY ABSORPTION XRAY

[6] Structural and mechanistic insights into methane oxidation by particulate methane monooxygenase [J].

Balasubramanian, Ramakrishnan ;

Rosenzweig, Amy C. .

ACCOUNTS OF CHEMICAL RESEARCH, 2007, 40 (07) :573-580

[7] Oxidation of methane by a biological dicopper centre [J].

Balasubramanian, Ramakrishnan ;

Smith, Stephen M. ;

Rawat, Swati ;

Yatsunyk, Liliya A. ;

Stemmler, Timothy L. ;

Rosenzweig, Amy C. .

NATURE, 2010, 465 (7294) :115-U131

[8] Methane to methanol over copper mordenite: yield improvement through multiple cycles and different synthesis techniques [J].

Bozbag, Selmi E. ;

Alayon, Evalyn Mae C. ;

Pechacek, Jan ;

Nachtegaal, Maarten ;

Ranocchiari, Marco ;

van Bokhoven, Jeroen A. .

CATALYSIS SCIENCE & TECHNOLOGY, 2016, 6 (13) :5011-5022

[9] Controlled oxidation of hydrocarbons by the membrane-bound methane monooxygenase: The case for a tricopper cluster [J].

Chan, Sunney I. ;

Yu, Steve S. -F. .

ACCOUNTS OF CHEMICAL RESEARCH, 2008, 41 (08) :969-979

[10] CU K-EDGE X-RAY-ABSORPTION SPECTROSCOPIC STUDY ON THE OCTAHEDRALLY COORDINATED TRIVALENT COPPER IN THE PEROVSKITE-RELATED COMPOUNDS LA2LI0.5CU0.5O4 AND LACUO3 [J].

CHOY, JH ;

KIM, DK ;

HWANG, SH ;

DEMAZEAU, G .

PHYSICAL REVIEW B, 1994, 50 (22) :16631-16639

← 1 2 3 4 5 →