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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
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
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
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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.
中文翻译：
[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
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。
更新日期：2022-06-14
中文翻译：
[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
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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