Tracking Mechanistic Pathway of Photocatalytic CO2 Reaction at Ni Sites Using Operando, Time-Resolved Spectroscopy

Journal of the American Chemical Society
Yangguang HuYujie Xiong

Abstract

Harvesting solar energy for catalytic conversion of CO2 into valuable chemical fuels/feedstocks is an attractive yet challenging strategy to realize a sustainable carbon-cycle utilization. Homogeneous catalysts typically exhibit higher activity and selectivity as compared with heterogeneous counterparts, benefiting from their atomically dispersed catalytic sites and versatile coordination structures. However, it is still a "black box" how the coordination and electronic structures of catalysts dynamically evolve during the reaction, forming the bottleneck for understanding their reaction pathways. Herein, we demonstrate to track the mechanistic pathway of photocatalytic CO2 reduction using a terpyridine nickel(II) complex as a catalyst model. Integrated with a typical homogeneous photosensitizer, the catalytic system offers a high selectivity of 99% for CO2-to-CO conversion with turnover number and turnover frequency as high as 2.36 × 107 and 385.6 s-1, respectively. We employ operando and time-resolved X-ray absorption spectroscopy, in combination with other in situ spectroscopic techniques and theoretical computations, to track the intermediate species of Ni catalyst in the photocatalytic CO2 reduction reaction for the first ...Continue Reading

References

Oct 4, 2007·The Journal of Physical Chemistry. a·Mina ParkKwang S Kim
May 7, 2010·Physical Chemistry Chemical Physics : PCCP·John J RehrKevin Jorissen
Mar 21, 2013·Chemical Reviews·Christopher K PrierDavid W C MacMillan
Mar 22, 2014·Physical Chemistry Chemical Physics : PCCP·Noémie ElgrishiMarc Fontecave
Jul 28, 2016·Journal of the American Chemical Society·Dooshaye MoonshiramStephen H Southworth
Dec 23, 2016·Journal of the American Chemical Society·Kyung Min ChoiOmar M Yaghi
Jan 14, 2017·Chemical Society Reviews·Noémie ElgrishiMarc Fontecave
Apr 4, 2017·Chemical Society Reviews·Chao GaoYujie Xiong
May 4, 2017·Journal of the American Chemical Society·Moritz F KuehnelErwin Reisner
Sep 19, 2018·Proceedings of the National Academy of Sciences of the United States of America·Irina V ChernyshovaSathish Ponnurangam
Nov 9, 2018·Journal of the American Chemical Society·Xiaofeng CuiYujie Xiong
Feb 3, 2019·The Journal of Chemical Physics·Shan JiangHolger Dau
May 2, 2019·ACS Central Science·Jeffrey M Barlow, Jenny Y Yang

❮ Previous
Next ❯

Citations

Aug 14, 2020·Chemical Society Reviews·Tingting KongYujie Xiong
Jul 27, 2021·The Journal of Physical Chemistry Letters·Yucheng YuanOu Chen
Aug 24, 2021·ACS Applied Materials & Interfaces·Qian LiangZhenhui Kang

❮ Previous
Next ❯

Related Concepts

Trending Feeds

COVID-19

Coronaviruses encompass a large family of viruses that cause the common cold as well as more serious diseases, such as the ongoing outbreak of coronavirus disease 2019 (COVID-19; formally known as 2019-nCoV). Coronaviruses can spread from animals to humans; symptoms include fever, cough, shortness of breath, and breathing difficulties; in more severe cases, infection can lead to death. This feed covers recent research on COVID-19.

Blastomycosis

Blastomycosis fungal infections spread through inhaling Blastomyces dermatitidis spores. Discover the latest research on blastomycosis fungal infections here.

Nuclear Pore Complex in ALS/FTD

Alterations in nucleocytoplasmic transport, controlled by the nuclear pore complex, may be involved in the pathomechanism underlying multiple neurodegenerative diseases including Amyotrophic Lateral Sclerosis and Frontotemporal Dementia. Here is the latest research on the nuclear pore complex in ALS and FTD.

Applications of Molecular Barcoding

The concept of molecular barcoding is that each original DNA or RNA molecule is attached to a unique sequence barcode. Sequence reads having different barcodes represent different original molecules, while sequence reads having the same barcode are results of PCR duplication from one original molecule. Discover the latest research on molecular barcoding here.

Chronic Fatigue Syndrome

Chronic fatigue syndrome is a disease characterized by unexplained disabling fatigue; the pathology of which is incompletely understood. Discover the latest research on chronic fatigue syndrome here.

Evolution of Pluripotency

Pluripotency refers to the ability of a cell to develop into three primary germ cell layers of the embryo. This feed focuses on the mechanisms that underlie the evolution of pluripotency. Here is the latest research.

Position Effect Variegation

Position Effect Variagation occurs when a gene is inactivated due to its positioning near heterochromatic regions within a chromosome. Discover the latest research on Position Effect Variagation here.

STING Receptor Agonists

Stimulator of IFN genes (STING) are a group of transmembrane proteins that are involved in the induction of type I interferon that is important in the innate immune response. The stimulation of STING has been an active area of research in the treatment of cancer and infectious diseases. Here is the latest research on STING receptor agonists.

Microbicide

Microbicides are products that can be applied to vaginal or rectal mucosal surfaces with the goal of preventing, or at least significantly reducing, the transmission of sexually transmitted infections. Here is the latest research on microbicides.