[Pt(OH)4(H2O)2] 的硫酸溶液：铂形态调查和实用的水合 Pt(IV) 氧化物形成,Inorganic Chemistry

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[Pt(OH)4(H2O)2] 的硫酸溶液：铂形态调查和实用的水合 Pt(IV) 氧化物形成
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2022-06-14 , DOI: 10.1021/acs.inorgchem.2c01134
Danila Vasilchenko ₁ , Pavel Tkachenko _{1,

2} , Sergey Tkachev ₁ , Pavel Popovetskiy ₁ , Vladislav Komarov ₁ , Tatyana Asanova ₁ , Igor Asanov ₁ , Evgeny Filatov ₁ , Eugene Maximovskiy ₁ , Evgeny Gerasimov ₃ , Angelina Zhurenok ₃ , Ekaterina Kozlova ₃

Affiliation

_{采用多种方法对氢氧化铂(IV){[Pt(OH) 4} (H ₂ O) ₂ ], HHPA}的硫酸溶液中的铂形态进行了系统研究。根据主要的 Pt 形式，标记了 H ₂ SO ₄浓度的三个区域： (1) 高达 3 MH ₂ SO ₄形成不稳定溶液，逐渐产生 PtO ₂ · x H ₂ O 颗粒；(2) 4–12 MH ₂ SO ₄，其中一系列单核水-硫酸根络合物 ([Pt(SO ₄ ) _n (H ₂ O)_{6– n} ] ^{4–2 n}，其中n = 0···4) 占主导地位；(3) 12 M 及以上，其中，与 [Pt(SO ₄ ) _n (H ₂ O) _{6- n} ] ^{4-2 n}物种一起，多核 Pt(IV) 物种和具有双齿配位模式的配合物形成硫酸根配体。水-羟基 Pt(IV) 阳离子 [Pt(OH) ₂ (H ₂ O) ₄ ]SO ₄（三斜晶相和单斜晶相）的盐类首次被分离并通过多种方法进行研究，包括单晶X射线衍射。PtO ₂的形成·研究了 HHPA 硫酸溶液 (1–3 M) 中的x H _{2 O 颗粒及其光谱特征和形态。}_{PtO 2} · x H ₂ O的沉积被强调为制备各种含Pt 多相催化剂的简便方法。_{Pt/gC 3} N ₄催化剂的制备证明了这种可能性，该催化剂在可见光照射下表现出优异的催化H _{2生成性能，量子效率高达5%，H}₂释放速率高达6.2 mol· h ^–1每克负载的铂。

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Sulfuric Acid Solutions of [Pt(OH)4(H2O)2]: A Platinum Speciation Survey and Hydrated Pt(IV) Oxide Formation for Practical Use

The systematic study of the platinum speciation in sulfuric acid solutions of platinum (IV) hydroxide {[Pt(OH)₄(H₂O)₂], HHPA} was performed with the use of a combination of methods. Depending on the prevailing Pt form, the three regions of H₂SO₄ concentration were marked: (1) up to 3 M H₂SO₄ forms unstable solutions gradually generating the PtO₂·xH₂O particles; (2) 4–12 M H₂SO₄, where the series of mononuclear aqua–sulfato complexes ([Pt(SO₄)_n(H₂O)_6–n]^4–2n, where n = 0···4) dominate; and (3) 12 M and above, where, along with [Pt(SO₄)_n(H₂O)_6–n]^4–2n species, the polynuclear Pt(IV) species and complexes with a bidentate coordination mode of the sulfato ligand are formed. For the first time, the salts of the aqua–hydroxo Pt(IV) cation [Pt(OH)₂(H₂O)₄]SO₄ (triclinic and monoclinic phases) were isolated and studied with a combination of methods, including the single-crystal X-ray diffraction. The formation of PtO₂·xH₂O particles in sulfuric acid solutions (1–3 M) of HHPA and their spectral characteristics and morphology were studied. The deposition of PtO₂·xH₂O was highlighted as a convenient method to prepare various Pt-containing heterogeneous catalysts. This possibility was illustrated by the preparation of Pt/g-C₃N₄ catalysts, which show an excellent performance in catalytic H₂ generation under visible light irradiation with a quantum efficiency up to 5% and a rate of H₂ evolution up to 6.2 mol·h^–1 per gram of loaded platinum.

更新日期：2022-06-14

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