Spectroscopic elucidation of energy transfer in hybrid inorganic?biological organisms for solar-to-chemical production [electronic resource]

 0 Người đánh giá. Xếp hạng trung bình 0

Tác giả:

Ngôn ngữ: eng

Ký hiệu phân loại: 333.79 Energy

Thông tin xuất bản: Washington, D.C. : Oak Ridge, Tenn. : United States. Dept. of Energy. Office of Science ; Distributed by the Office of Scientific and Technical Information, U.S. Dept. of Energy, 2016

Mô tả vật lý: Size: p. 11750-11755 : , digital, PDF file.

Bộ sưu tập: Metadata

ID: 255766

 We present that the rise of inorganic?biological hybrid organisms for solar-to-chemical production has spurred mechanistic investigations into the dynamics of the biotic?abiotic interface to drive the development of next-generation systems. The model system, Moorella thermoacetica?cadmium sulfide (CdS), combines an inorganic semiconductor nanoparticle light harvester with an acetogenic bacterium to drive the photosynthetic reduction of CO<
 sub>
 2<
 /sub>
  to acetic acid with high efficiency. In this work, we report insights into this unique electrotrophic behavior and propose a charge-transfer mechanism from CdS to M. thermoacetica. Transient absorption (TA) spectroscopy revealed that photoexcited electron transfer rates increase with increasing hydrogenase (H<
 sub>
 2<
 /sub>
 ase) enzyme activity. On the same time scale as the TA spectroscopy, time-resolved infrared (TRIR) spectroscopy showed spectral changes in the 1,700?1,900-cm<
 sup>
 -1<
 /sup>
  spectral region. The quantum efficiency of this system for photosynthetic acetic acid generation also increased with increasing H<
 sub>
 2<
 /sub>
 ase activity and shorter carrier lifetimes when averaged over the first 24 h of photosynthesis. However, within the initial 3 h of photosynthesis, the rate followed an opposite trend: The bacteria with the lowest H<
 sub>
 2<
 /sub>
 ase activity photosynthesized acetic acid the fastest. These results suggest a two-pathway mechanism: a high quantum efficiency charge-transfer pathway to H<
 sub>
 2<
 /sub>
 ase generating H<
 sub>
 2<
 /sub>
  as a molecular intermediate that dominates at long time scales (24 h), and a direct energy-transducing enzymatic pathway responsible for acetic acid production at short time scales (3 h). Lastly, this work represents a promising platform to utilize conventional spectroscopic methodology to extract insights from more complex biotic?abiotic hybrid systems.
Tạo bộ sưu tập với mã QR

THƯ VIỆN - TRƯỜNG ĐẠI HỌC CÔNG NGHỆ TP.HCM

ĐT: (028) 71010608 | Email: tt.thuvien@hutech.edu.vn

Copyright @2024 THƯ VIỆN HUTECH