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Title: Light-Gated Synthetic Protocells for Plasmon-Enhanced Chemiosmotic Gradient Generation and ATP Synthesis

Abstract

We present a light-gated protocell model made of plasmonic colloidal capsules (CCs) assembled with bacteriorhodopsin for converting solar energy into electrochemical gradients to drive the synthesis of energy-storage molecules. This synthetic protocell incorporated an important intrinsic property of noble metal colloidal particles, namely, plasmonic resonance. In particular, the near-field coupling between adjacent metal nanoparticles gave rise to strongly localized electric fields and resulted in a broad absorption in the whole visible spectra, which in turn promoted the flux of photons to bacteriorhodopsin and accelerated the proton pumping kinetics. The cell-like potential of this design was further demonstrated by leveraging the outward pumped protons as “chemical signals” for triggering ATP biosynthesis in a coexistent synthetic protocell population. Hereby, we lay the ground work for the engineering of colloidal supraparticle-based synthetic protocells with higher-order functionalities.

Authors:
 [1];  [1]; ORCiD logo [1];  [2]; ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Applied Materials Division
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Biosciences Division
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); ANL Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1509999
Alternate Identifier(s):
OSTI ID: 1495285
Grant/Contract Number:  
AC02-06CH11357; AC02- 06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 58; Journal Issue: 15; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
59 BASIC BIOLOGICAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; bacteriorhodopsin; chemiosmotic gradients; colloidal capsules; plasmonic resonance; protocells

Citation Formats

Chen, Zhaowei, De Queiros Silveira, Gleiciani, Ma, Xuedan, Xie, Yunsong, Wu, Yimin A., Barry, Edward, Rajh, Tijana, Fry, H. Christopher, Laible, Philip D., and Rozhkova, Elena A. Light-Gated Synthetic Protocells for Plasmon-Enhanced Chemiosmotic Gradient Generation and ATP Synthesis. United States: N. p., 2019. Web. doi:10.1002/anie.201813963.
Chen, Zhaowei, De Queiros Silveira, Gleiciani, Ma, Xuedan, Xie, Yunsong, Wu, Yimin A., Barry, Edward, Rajh, Tijana, Fry, H. Christopher, Laible, Philip D., & Rozhkova, Elena A. Light-Gated Synthetic Protocells for Plasmon-Enhanced Chemiosmotic Gradient Generation and ATP Synthesis. United States. doi:10.1002/anie.201813963.
Chen, Zhaowei, De Queiros Silveira, Gleiciani, Ma, Xuedan, Xie, Yunsong, Wu, Yimin A., Barry, Edward, Rajh, Tijana, Fry, H. Christopher, Laible, Philip D., and Rozhkova, Elena A. Wed . "Light-Gated Synthetic Protocells for Plasmon-Enhanced Chemiosmotic Gradient Generation and ATP Synthesis". United States. doi:10.1002/anie.201813963. https://www.osti.gov/servlets/purl/1509999.
@article{osti_1509999,
title = {Light-Gated Synthetic Protocells for Plasmon-Enhanced Chemiosmotic Gradient Generation and ATP Synthesis},
author = {Chen, Zhaowei and De Queiros Silveira, Gleiciani and Ma, Xuedan and Xie, Yunsong and Wu, Yimin A. and Barry, Edward and Rajh, Tijana and Fry, H. Christopher and Laible, Philip D. and Rozhkova, Elena A.},
abstractNote = {We present a light-gated protocell model made of plasmonic colloidal capsules (CCs) assembled with bacteriorhodopsin for converting solar energy into electrochemical gradients to drive the synthesis of energy-storage molecules. This synthetic protocell incorporated an important intrinsic property of noble metal colloidal particles, namely, plasmonic resonance. In particular, the near-field coupling between adjacent metal nanoparticles gave rise to strongly localized electric fields and resulted in a broad absorption in the whole visible spectra, which in turn promoted the flux of photons to bacteriorhodopsin and accelerated the proton pumping kinetics. The cell-like potential of this design was further demonstrated by leveraging the outward pumped protons as “chemical signals” for triggering ATP biosynthesis in a coexistent synthetic protocell population. Hereby, we lay the ground work for the engineering of colloidal supraparticle-based synthetic protocells with higher-order functionalities.},
doi = {10.1002/anie.201813963},
journal = {Angewandte Chemie (International Edition)},
number = 15,
volume = 58,
place = {United States},
year = {2019},
month = {1}
}

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    Light‐Driven Active Proton Transport through Photoacid‐ and Photobase‐Doped Janus Graphene Oxide Membranes
    journal, June 2019


    Light‐Driven Active Proton Transport through Photoacid‐ and Photobase‐Doped Janus Graphene Oxide Membranes
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