Рис. 1. Схема получения прямоугольных мицелл толщиной 20 нм с контролируемой площадью поверхности. Структура получается путем добавления блочного сополимера (БСП) с короткой полукристалличной частью (полиферроценилсилан, ПФС) в смеси с чистым ПФС к коротким циллиндрическим мицеллам на основе ПФС. Рисунок из обсуждаемой статьи в Science

Британским и канадским химикам впервые удалось методом самосборки получить двумерные прямоугольные наноструктуры при полном контроле над площадью и химическим составом их поверхности. Успех был достигнут за счет использования блочных сополимеров с полукристаллическим блоком, нахождения нужного отношения длины блоков и добавления в раствор свободных цепочек полукристаллического полимера. Эта технология может в будущем пригодиться для использования во флуоресцентной томографии, наноэлектронике, катализе, жидких кристаллax, подвижных нано- и микромашинax или терапевтических носителях.

В конце XX века стало понятно, что наноразмерные частицы (размером 1–100 нм как минимум в одном измерении) обладают свойствами, которые не проявляются в макромире. Происходит это потому, что при уменьшении размера частиц до наноуровня становится существенным вклад свойств поверхности в свойства объекта. Другой причиной изменения свойств является то, что на наноуровне проявляются законы квантовой механики. Так, когда в 2004 году группой физиков во главе с Андреем Геймом и Константином Новосёловым были получены первые образцы графена, оказалось, что такие двумерные структуры способны проявлять поразительные электронные свойства, качественно отличающиеся от всех прежде наблюдаемых. Сегодня сотни экспериментальных групп исследуют электронные свойства графена.

Классифицировать наночастицы легче всего по степени снижения размерности: двумерные — квантовые плоскости, одномерные — квантовые нити, нульмерные — квантовые точки. Весь спектр сниженных размерностей удобно объяснить на примере углеродных наночастиц (рис. 2).

Рис 2. Углеродные наночастицы. Слева направо: нульмерный фуллерен, одномерная углеродная нанотрубка, двумерный графен. Рисунок с сайта surrealsciencestuff.wordpress.com

Мир нанотехнологий, конечно, не ограничивается углеродом: почти любой наноразмерный материал по-своему необычен и потенциально интересен. Как же их получать? Для получения нульмерных наноматериалов (квантовых точек) подходят, как правило, известные химические методы, ведь квантовая точка — это обычно просто большая молекула. Для получения одно- и двумерных материалов требовались новые подходы. Следует отметить, что в тех измерениях, в которых материал не наноразмерен (где его размерность больше 100 нм), есть теоретическая возможность чередовать состав поверхности и таким образом получать еще более интересные материалы для разных применений. Однако модифицировать графен и другие подобные материалы очень сложно химически. Создание двумерных наноструктур с контролируемыми размерами и химическим составом поверхности — одна из нерешенных задач нанотехнологии. С открытием графена эта область исследований получила серьезный толчок, но, не считая нескольких примеров, проблема оставалась нерешенной по сей день.

Самосборка макромолекул в растворе — наиболее элегантный, удобный и экономичный метод получения наноматериалов, и именно этим методом теоретически можно создавать структуры с контролируемым составом поверхности, если чередовать макромолекулы, которые добавляют в раствор.

Группа ученых из Бристольского университета (Великобритания) и Торонтского университета (Канада), воодушевленная своим недавним успехом в контроле над одномерными наноструктурами (см. Появился способ получения нецентросимметричных наночастиц, «Элементы», 17.08.2012), достигнутым с помощью самосборки блочных сополимеров (БСП), в котором одним из блоков был полукристаллический полиферроценилсилан (ПФС), попробовала использовать подобный подход для получения двумерных наноструктур.

Напомним, что БСП — это полимер, в котором две части (два блока) или более состоят из разных мономеров. Самосборка блочных сополимеров в растворе происходит за счет разной растворимости двух частей. Полукристалличность — это способность полимера кристаллизоваться, то есть упорядоченно складываться. Приставка «полу-» здесь необходима, потому что при складывании полимера в кристалл всегда остаются некристалличесткие (аморфные) фрагменты.

Рис 3. Полимеры, упоминаемые в тексте, в порядке их появления. Числовой индекс n у названия полимера означает степень полимеризации — усредненное число мономерных звеньев в молекуле полимера. Азот на кольце пиридина в П2ВП способен связываться с металлами и некоторыми другими молекулами — свойство, которое было использовано авторами статьи (см. ниже в тексте)

Успех с одномерными структурами был обусловлен тем, что полукристаллическая часть блочного сополимера была намного короче растворимой части. При самосборке длинные растворимые цепочки БСП на поверхности образуемой мицеллы, мешая друг другу, не позволяли создать плоскую структуру, и получалась нить. При укорачивании растворимой цепочки в БСП мицеллы или не получались вовсе или выпадали в осадок.

Тогда решили поэкспериментировать с самосборкой смеси БСП с длинной растворимой частью и чистого полиферроценилсилана (ПФС). Идея заключалась в том, что дополнительные цепочки ПФС, сокристаллизуясь с блоком ПФС в сополимере, должный создать дополнительную площадь поверхности, позволив растворимым цепочкам не мешать друг другу. Смесь добавляли к раствору коротких нитевидных мицелл, чтобы те служили центром кристаллизации.

После нескольких неудачных попыток опыты со смесями ПФС28–ПДМС560/ПФС20 и ПФС38–П2ВП502/ПФС20 попали в точку (рис. 4). Добавление полимеров в раствор с короткими мицеллами привело к возникновению прямоугольных структур высотой ~20 нм, причем их размер (площадь) полностью контролировался количеством добавленого полимера. Так как края мицеллы не закрыты, можно добавлять еще блочного сополимера, и он будет без остатка прирастать к мицелле.

Рис. 4. А — схематическая репрезентация получения прямоугольных мицелл из смеси БСП/ПФС в соотношении 1:1 по весу. В — снимок прямоугольных мицелл, полученный с помощью просвечивающего электронного микроскопа (ПЭМ). С — снимок, полученный с помощью aтомно-силовогo микроскопa (АСМ). D — высота структуры, измерeнная АСМ. Цвет кривой соответствует цвету линии на рис. 4, С — в этом месте высота была измерена. Рисунок из обсуждаемой статьи в Science

Чтобы наглядно продемонстрировать контроль над площадью и химическим составом поверхности, авторы вырастили мицеллы, последовательно добавляя к первичной прямоугольной мицелле из ПФС–П2ВП полимеры с разными цветными (флуоресцентными) группами (рис. 5). Подробнее о цветных мицеллах и о том, зачем они нужны, можно прочитать здесь.

Рис. 5. Цветные прямоугольные мицеллы, полученные самосборкой путем последовательного добавления ПФС–ПДМС с привязанными молекулами флюоресцентных красителей. Верхний ряд — схематическая репрезентация; средний ряд — снимки с помощью конфокального микроскопа; нижний ряд — снимки отдельных мицелл, сделанные с помощью структурированной иллюминационной микроскопии (см. Structured illumination microscopy). Рисунок из обсуждаемой статьи в Science

Итак, авторы продемонстрировали возможность чередовать химический состав поверхности мицеллы. Как эту возможность использовать? Один из полимеров в составе мицеллы, использованный при самосборке, — П2ВП — способен связываться координативной связью с металлами. Добавив наночастицы платины диаметром 2 нм к раствору мицелл, чередующих на своей поверхности ПДМС и П2ВП, авторы селективно связали цепочки П2ВП, не затронув ПДМС. Иными словами, в области с П2ВП поверхность оказалось сшита наночастицами платины.

Добавив тетрагидрофуран (ТГФ), который в обычных условиях растворяет все ПФС-содержащие блочные сополимеры, авторы растворили только ПФС–ПДМС. После растворения получились нанорамки — прямоугольные мицеллы из сшитого П2ВП с отверстием в центре. Отверстия можно получать любого размера, в зависимости от величины блоков П2ВП и ПДМС (рис. 6). В мицеллах с самым широким отверстием толщина боковых стенок <100 нм — это фактически циклический гибрид одномерного и двумерного наноматериала.

Рис. 6. Получение нанорамок. Первичная структура состоит из ПФС–ПДМС. На нее наращивается слой ПФС–П2ВП, который позже селективно сшивается наночастицами платины. Растворение несшитой центральной части в тетрагидрофуране (ТГФ) дает нанорамку. Вверху — схематическое изображение процесса. Внизу — снимки нанорамок с разной величиной отверстий, выполненные при помощи просвечивающего электронного микроскопа (ПЭМ). Рисунок из обсуждаемой статьи в Science

Овладев технологией, авторы проделали еще много опытов для демонстрации ее силы:

В частицах диоксида кремния есть фрагменты SiOH, которые образуют водородные связи с пиридинами в П2ВП. На рис. 7, С видно, что наночастицы (черные точки) селективно прикреплены к блоку мицеллы с П2ВП.

Рис. 7. А — снимок мицелл из восьми чередующихся блоков ПФС–ПДМС и ПФС–П2ВП. В — снимок мицеллы из трех разных блоков (в порядке от центра: ПФС–ПБМА, ПФС–ПДМС, ПФС–П2ВП). С — снимок мицеллы из ПФС–ПДМС и ПФС–П2ВП, обработанные наночастицами диоксида кремния (70 нм), приставшими селективно к П2ВП благодаря водородным связям. D — снимок мицеллы длинной более 60 мкм и шириной более 20 мкм, сделанный при помощи aтомно-силовогo микроскопa (АСМ). E — снимок мицелл, выложенных с помощью оптического пинцета в форме аббревиатуры UOB (вверху); снимок того же места сделанный с помощью конфокального микроскопа (внизу). F — сxематичecкое изображение манипуляции мицеллами с помощью оптического пинцета. Снимки A, B, C и E (вверху) сделаны при помощи просвечивающего электронного микроскопа (ПЭМ). Рисунок из обсуждаемой статьи в Science

Авторы статьи — химики и материаловеды — не ставили в этой работе задачи найти и продемонстрировать уникальные физические свойства полученных новых структур. Они уверены, что этой технологией заинтересуются физики и продолжат начатую революцию. Так как на сегодняшний день известны ПФС-содержащие блочные сополимеры с огромным количеством химических модификаций в растворимой части, можно получать наноструктуры, имеющие на поверхности всё что угодно: от биомолекул до полупроводников, от металлов доброй половины таблицы Менделеева до сложных молекулярных архитектур. Авторы отмечают, что технология можeт в будущем пригодиться для использования во флуоресцентной томографии, наноэлектронике, катализе, в жидких кристаллax, подвижных нано- и микромашинax или терапевтических носителяx. Места для фантазии много.

Источник: elementy.ru

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A) it is acceptable to use copyrighted material for economic gain as long as proper credit is given to the author.. . B) all original work located on the Internet is to be considered copyrighted.. . C) only items marked with the ? symbol are considered copyrighted.. . D) all Internet content is free for anyone to use..

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I’m developing a new blog concerning literary works (what I’ve reviewed, what I’m reading), but I’m having problem thinking about a title. I like the idea of something involving an obsession with literary works yet I believe bookophilia is on the ordinary side. What do you think about Litophilia? Is it also comparable to «lithophilia» Which means the love of stones? Any suggestions? Thanks!.

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I maintain several blogs & discussion forums and also permit people to create their comments on them. I inspect routinely as well as eliminate any swear words, etc. I additionally ask commentors not to leave any type of defamatory terms on the blogs/forums. Nevertheless, that stated, am i still legitimately responsible for the content on my blog/forums if they write a libelous comment or abusive remarks?. Numerous many thanks.

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