Remote Optically Controlled Modulation of Catalytic Properties of Nanoparticles through Reconfiguration of the Inorganic/Organic Interface

Lawrence, Randy L.; Scola, Billy; Li, Yue; Lim, Chang Keun; Liu, Yang; Prasad, Paras N.; Swihart, Mark T.; Knecht, Marc R.

doi:10.1021/acsnano.6b04555

Cited by 58 publications

(113 citation statements)

References 36 publications

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“…Such long half-lives are a result of stabilization of the MAM moiety on the Au surface, which can inhibit the thermally driven conformation change. 8 These results demonstrate that the reactivity observed from the NPs with the biointerface in the cis conformation arises from the anticipated configuration and that photoswitch thermal isomerization is not complicating the reactivity analysis.…”

Section: Resultsmentioning

confidence: 67%

“…Previous studies fully analyzed the AuBP1C-MAM-and MAM-CAuBP1-capped materials, which demonstrated nearly identical results. 8 Figure 1a specifically presents the analysis for Au NPs fabricated using the AuBP1[C-MAM]. For the peptide alone (red spectrum), two peaks were observed: one at 320 nm and a second at 450 nm.…”

Section: Resultsmentioning

confidence: 99%

“…In this manner, different catalytic capabilities can be achieved from the same Au NPs depending upon the peptide surface configuration. 8 For instance, using the reduction of 4-nitrophenol to 4-aminophenol as a model reaction, the reactivity for Au NPs capped with the AuBP1 peptide with the photoswitch at the N-terminus demonstrated notably higher activity with the azobenzene molecule in the trans conformation compared to the cis conformation.…”

Section: Introductionmentioning

confidence: 99%

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Optical Control of Nanoparticle Catalysis Influenced by Photoswitch Positioning in Hybrid Peptide Capping Ligands

Lawrence

Hughes

Cendan

et al. 2018

ACS Appl. Mater. Interfaces

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Here, we present an in-depth analysis of structural factors that modulate peptide-capped nanoparticle catalytic activity via optically driven structural reconfiguration of the biointerface present at the particle surface. Six different sets of peptide-capped Au nanoparticles were prepared, in which an azobenzene photoswitch was incorporated into one of two well-studied peptide sequences with known affinity for Au, each at one of three different positions: the N- or C-terminus or mid-sequence. Changes in the photoswitch isomerization state induce a reversible structural change in the surface-bound peptide, which modulates the catalytic activity of the material. This control of reactivity is attributed to changes in the amount of accessible metallic surface area available to drive the reaction. This research specifically focuses on the effect of the peptide sequence and photoswitch position in the biomolecule, from which potential target systems for on/off reactivity have been identified. Additionally, trends associated with photoswitch position for a peptide sequence (Pd4) have been identified. Integrating the azobenzene at the N-terminus or central region results in nanocatalysts with greater reactivity in the trans and cis conformations, respectively, however, positioning the photoswitch at the C-terminus gives rise to a unique system that is reactive in the trans conformation and partially deactivated in the cis conformation. These results provide a fundamental basis for new directions in nanoparticle catalyst development to control activity in real time, which could have significant implications in the design of catalysts for multistep reactions using a single catalyst. Additionally, such a fine level of interfacial structural control could prove to be important for applications beyond catalysis, including biosensing, photonics, and energy technologies that are highly dependent on particle surface structures.

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Section: Resultsmentioning

confidence: 67%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Optical Control of Nanoparticle Catalysis Influenced by Photoswitch Positioning in Hybrid Peptide Capping Ligands

Lawrence

Hughes

Cendan

et al. 2018

ACS Appl. Mater. Interfaces

Self Cite

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“…All these properties have been widely exploited for the preparation of different types of smart materials, and it is possible to find in the literature interesting examples related to smart catalysis. Lawrence et al [44] proposed the use of peptide-ligand-capped Au NPs with azobenzene units integrated into the biomolecular ligand for the switchable catalysis of the reduction of 4-nitrophenol by NaBH 4 . Illumination of the system with UV light causes the isomerization of the azobenzene units of the ligand from the trans to the cis form.…”

Section: Light-controlled Switchable Catalysismentioning

confidence: 99%

Switchable Stimuli-Responsive Heterogeneous Catalysis

Vassalini

Alessandri

2018

Catalysts

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Heterogeneous catalytic systems based on the use of stimuli-responsive materials can be switched from an "on" active state to an "off" inactive state, which contributes to endowing the catalysts with unique functional properties, such as adaptability, recyclability and precise spatial and temporal control on different types of chemical reactions. All these properties constitute a step toward the development of nature-inspired catalytic systems. Even if this is a niche area in the field of catalysis, it is possible to find in literature intriguing examples of dynamic catalysts, whose systematic analysis and review are still lacking. The aim of this work is to examine the recent developments of stimuli-responsive heterogeneous catalytic systems from the viewpoint of different approaches that have been proposed to obtain a dynamic control of catalytic efficiency. Because of the variety of reactions and conditions, it is difficult to make a quantitative comparison between the efficiencies of the considered systems, but the analysis of the different strategies can inspire the preparation of new smart catalytic systems.Catalysts 2018, 8, 569 2 of 25 fields [6] and mechanical stress [7], have also been exploited. A large variability can also be observed in the type of system response: variations of chemical properties, solubility, shape, volume, color, aggregation state, electrical properties, magnetic properties, mechanical properties, etc. are all possible. Thanks to this high versatility, artificial smart materials have found application in various sectors [8], ranging from medicine to national security and structural engineering [9]. They are commonly employed for drug delivery [10], self-healing [11], sensing [12], actuations [13], information storage [14], etc. Their use for catalytic purposes has been remarkably less investigated, even if heterogeneous catalysis can fully take advantage of the dynamic behavior of smart materials. For example, it is possible to make a catalyst to pass from a state of activity (an "on" state) to a state of inertness (an "off" state) in a controlled way, with a precise temporal control, obtaining switchable catalysis. In other circumstances, the possibility of modulating the reaction rate in a continuous way, regulating the amount of accessible active sites and accelerating or lowering the reaction rate in a non-discrete way, is more interesting, and in this case we can also exploit stimuli-responsive materials. It is also possible to create microenvironments in which the reaction occurs preferentially, accomplishing a spatial control on the reaction development. In addition, the responsiveness of the employed systems can be exploited to improve the recyclability of the catalytic system, making the catalyst separation from the reaction medium and its reuse easier.In this review, we analyze some of the latest works on dynamic systems in the field of heterogeneous catalysis. Many more examples can be found for homogeneous catalysis, but most of them have been already analyzed in previ...

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“…Herein, we report a uniform bilayer configuration made of Au nanorods embedded in graphene oxide (AuNRs@GO) and poly(methyl methacrylate) (PMMA), enabling a light‐sensitive artificial muscle to perform complex limb‐like motions without joints literally. Such “holistic artificial muscle” (HAM) tailors the promising nature of light‐responsive materials, leading to control the strength of contraction/expansion through the plasmonic‐assisted actuation under laser exposure with different wavelength.…”

mentioning

confidence: 99%

Plasmonic‐Assisted Graphene Oxide Artificial Muscles

et al. 2018

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Muscles and joints make highly coordinated motion, which can be partly mimicked to drive robots or facilitate activities. However, most cases primarily employ actuators enabling simple deformations. Therefore, a mature artificial motor system requires many actuators assembled with jointed structures to accomplish complex motions, posing limitations and challenges to the fabrication, integration, and applicability of the system. Here, a holistic artificial muscle with integrated light‐addressable nodes, using one‐step laser printing from a bilayer structure of poly(methyl methacrylate) and graphene oxide compounded with gold nanorods (AuNRs), is reported. Utilizing the synergistic effect of the AuNRs with high plasmonic property and wavelength‐selectivity as well as graphene with good flexibility and thermal conductivity, the artificial muscle can implement full‐function motility without further integration, which is reconfigurable through wavelength‐sensitive light activation. A biomimetic robot and artificial hand are demonstrated, showcasing functionalized control, which is desirable for various applications, from soft robotics to human assists.

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Remote Optically Controlled Modulation of Catalytic Properties of Nanoparticles through Reconfiguration of the Inorganic/Organic Interface

Cited by 58 publications

References 36 publications

Optical Control of Nanoparticle Catalysis Influenced by Photoswitch Positioning in Hybrid Peptide Capping Ligands

Optical Control of Nanoparticle Catalysis Influenced by Photoswitch Positioning in Hybrid Peptide Capping Ligands

Switchable Stimuli-Responsive Heterogeneous Catalysis

Plasmonic‐Assisted Graphene Oxide Artificial Muscles

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