本文選題：單原子催化劑 + 非貴金屬��； 參考：《催化學(xué)報(bào)》2017年09期

【摘要】：由于良好的催化活性和穩(wěn)定性,貴金屬催化劑已經(jīng)被廣泛應(yīng)用于各種異相催化反應(yīng)中,但是貴金屬的稀有性和高成本無法滿足未來日益增長的催化需求.2011年,張濤課題組成功地制備了高效、穩(wěn)定的鉑單原子催化劑.高效的單原子催化劑利用單個(gè)活性位點(diǎn)作為催化活性中心,可能會(huì)成為連接同相催化和異相催化的橋梁.然而從經(jīng)濟(jì)適用的長遠(yuǎn)角度考慮,將非貴金屬催化劑縮小到原子尺度是否也會(huì)展現(xiàn)出優(yōu)良的催化活性;是否有潛力替代目前已被廣泛應(yīng)用的貴金屬催化劑?雖然現(xiàn)階段非貴金屬催化劑的催化性能仍無法達(dá)到貴金屬催化劑的標(biāo)準(zhǔn),但是已有相關(guān)研究從理論和實(shí)驗(yàn)上報(bào)道了非貴金屬單原子催化劑及其優(yōu)異的性能表明了其在未來發(fā)展中極其重要,因而,可以預(yù)見這兩個(gè)疑問的答案都是肯定的.單原子概念的出現(xiàn)不僅為提高貴金屬的催化性能及成本的降低指明了方向,同時(shí)也為制備具有高催化活性、甚至可與貴金屬催化劑相媲美的非貴金屬催化劑提供了可能性.我們?cè)谏鲜霰尘跋?闡述了對(duì)單原子的概念日益加深的機(jī)制認(rèn)知,并從理論和實(shí)驗(yàn)上概述了非貴金屬單原子催化劑近期的發(fā)展情況,指出了目前的在單原子催化劑領(lǐng)域需要解決的一些問題,最后,針對(duì)研究現(xiàn)狀,我們對(duì)未來單原子的發(fā)展提出了相應(yīng)的展望.單原子催化劑具有較高的表面能,因而,如何尋找合適的基體與單原子相互作用,進(jìn)而,使基體材料像一只手一樣穩(wěn)固地"抓緊"單原子,因而,降低其高表面能則是發(fā)揮優(yōu)良催化性能的基礎(chǔ).強(qiáng)金屬 基體相互作用(SMSI)不僅可以將單原子限制在基體表面,亦會(huì)影響整個(gè)催化過程.目前應(yīng)用于單原子催化劑的基體種類很多,如金屬氧化物、金屬以及其他材料,而對(duì)SMSI認(rèn)知?jiǎng)t主要分兩大類,一類是源自于基體表面的結(jié)構(gòu)缺陷,另一類是源于其電子缺陷.從目前的發(fā)展?fàn)顩r來看SMSI機(jī)制仍有很多疑惑尚未解決,例如對(duì)電子轉(zhuǎn)移影響的認(rèn)知等.理論研究表明,在某些反應(yīng)中非貴金屬單原子展示出可替代貴金屬的催化性質(zhì).比如,在一氧化碳優(yōu)先反應(yīng)(PROX)中,單原子鈷和鈦展示出的催化性能可與貴金屬相媲美;理論計(jì)算同樣證明單原子鎳在一氧化碳還原中的催化活性比單原子銥優(yōu)秀,甚至與單原子鉑類似.大量的實(shí)驗(yàn)進(jìn)展也報(bào)道了非貴金屬單原子同樣能在其他反應(yīng)中展現(xiàn)出優(yōu)異的性能,如氧析出反應(yīng)(OER)、氫析出反應(yīng)(HER)和氧還原反應(yīng)(ORR).對(duì)于單原子催化劑,還有很多問題需要我們?nèi)ソ鉀Q,例如基體對(duì)于催化過程的具體影響、非貴金屬的電子結(jié)構(gòu)對(duì)于其催化性能的影響,以及單原子在基體上產(chǎn)生相互作用的位點(diǎn)等問題.縱然有許多問題需要更加深入的研究,但是單原子概念的出現(xiàn),使得非貴金屬催化劑材料取代傳統(tǒng)貴金屬催化劑成為了可能.
[Abstract]:Due to their good catalytic activity and stability, noble metal catalysts have been widely used in various heterogeneous catalytic reactions, but the rare and high cost of precious metals can not meet the increasing demand for catalysis in the future. High efficient and stable platinum monatomic catalysts were successfully prepared by Zhang Tao team. The highly efficient monoatomic catalyst uses a single active site as the catalytic active center, which may become the bridge between the same phase catalysis and heterogeneous catalysis. However, from the long-term perspective of economic application, whether the reduction of non-noble metal catalysts to atomic scale will also show good catalytic activity, and whether it has the potential to replace the precious metal catalysts that have been widely used at present? Although the catalytic performance of non-noble metal catalyst is still not up to the standard of noble metal catalyst, However, relevant studies have reported theoretically and experimentally that non-precious metal monatomic catalysts and their excellent properties show that they are extremely important in the future development. Therefore, the answer to these two questions can be predicted to be yes. The appearance of monatomic concept not only indicates the direction of improving the catalytic performance and cost reduction of noble metals, but also provides the possibility for the preparation of non-noble metal catalysts with high catalytic activity and even comparable with noble metal catalysts. Under the above background, we expound the increasing understanding of the mechanism of the concept of single atom, and summarize the recent development of non-noble metal monatomic catalysts, both theoretically and experimentally. Some problems that need to be solved in the field of monatomic catalysts are pointed out. Finally, in view of the present research situation, we put forward the corresponding prospects for the development of monatomic catalysts in the future. Monatomic catalysts have high surface energy, so how to find the appropriate matrix to interact with the single atom, so that the matrix material can "grasp" the single atom as firmly as a hand, so, The reduction of its high surface energy is the basis for its excellent catalytic performance. The strong metal matrix interaction (SMSI) can not only limit the single atom to the substrate surface, but also affect the whole catalytic process. At present, there are many kinds of monatomic catalysts, such as metal oxides, metals and other materials. The cognition of SMSI is mainly divided into two categories, one is the structural defects derived from the substrate surface, the other is the electronic defects. From the current development situation, there are still many doubts about the SMSI mechanism, such as the understanding of the effect of electron transfer. Theoretical studies show that in some reactions, the non-noble metal monoatom exhibits the catalytic properties of substituted noble metals. For example, in the carbon monoxide preferential reaction (Prox), monoatomic cobalt and titanium exhibit catalytic properties comparable to those of precious metals, and theoretical calculations also prove that monatomic nickel has better catalytic activity than monatomic iridium in carbon monoxide reduction. Even monatomic platinum is similar. A large number of experimental advances have also been reported that non-noble metal monatoms can also exhibit excellent properties in other reactions, such as oxygen precipitation reaction, hydrogen precipitation reaction and oxygen reduction reaction. For monatomic catalysts, there are still many problems to be solved, such as the specific effect of the matrix on the catalytic process, and the influence of the electronic structure of the non-noble metal on its catalytic performance. The interaction sites of monatomic atoms on the matrix are also discussed. Although there are many problems that need to be further studied, the concept of single atom makes it possible for non-precious metal catalyst materials to replace traditional noble metal catalysts.
【作者單位】： 吉林大學(xué)汽車仿真與控制國家重點(diǎn)實(shí)驗(yàn)室和材料科學(xué)與工程學(xué)院;西班牙能源協(xié)作研究中心;西班牙巴斯克科學(xué)基金會(huì);
【基金】：國家自然科學(xué)基金(51372095) 吉林大學(xué)學(xué)術(shù)帶頭人專項(xiàng)基金(419080500630)
【分類號(hào)】：O643.36

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