氢氧直接合成过氧化氢用催化剂的研究进展

doi:10.16085/j.issn.1000-6613.2020-2176

摘要/Abstract

摘要：

过氧化氢（H₂O₂）是一种高效的绿色氧化剂，广泛应用于化学品合成、印染纺织、污水处理等领域。近年来，氢氧直接合成过氧化氢作为一种简单、环保、原子效率高的合成方法，成为一大研究热点。本文系统性地介绍了近年来氢氧直接合成过氧化氢催化剂的催化反应机理，负载金属的不同结构和性质对直接合成过氧化氢的催化性能与作用机理，重点讨论了与催化剂载体相关的载体结构、载体酸性、载体添加物、载体与金属相互作用等方面对反应活性和选择性的影响。最后对比了近年来直接合成过氧化氢用催化剂的催化性能，认为合成高选择性、高产率的催化剂仍是未来直接合成过氧化氢工业化应用的发展方向。

关键词: 过氧化氢, 直接合成, 催化剂, 贵金属催化, 催化剂载体

Abstract:

Hydrogen peroxide (H₂O₂) is a green oxidant with high efficiency (above 47.1% active oxygen), and is widely used in the production of fine chemicals, bleaching of textile and pulp, treatment of wastewater, and green chemical synthesis metallurgy. Recently, the direct synthesis of H₂O₂ (DSHP) from H₂ and O₂ has attracted great attention because of its environmentally friendly process and simple, atom-efficient route. In this paper, the catalytic mechanism for DSHP and the influence of catalytic performance for different structures and properties of different metals in recent years are summarized. The support acid sites, support structure, the interaction between active sites and acid sites are discussed. Finally, the catalytic performance of catalysts for DSHP in recent years are compared. It reveals that the industrial application of catalysts for DSHP with high selectivity and high productivity in the future is still the development direction.

Key words: hydrogen peroxide, direct synthesis, catalyst, noble metal catalysis, catalysts support

中图分类号:

TQ123.6

梁海瑞, 王涖, 刘国柱. 氢氧直接合成过氧化氢用催化剂的研究进展[J]. 化工进展, 2021, 40(4): 2060-2069.

LIANG Hairui, WANG Li, LIU Guozhu. A review of recent development on catalysts for direct synthesis of hydrogen peroxide from hydrogen and oxygen[J]. Chemical Industry and Engineering Progress, 2021, 40(4): 2060-2069.

图/表 6

参考文献 46

1	CIRIMINNA R, ALBANESE L, MENEGUZZO F, et al. Hydrogen peroxide: a key chemical for today's sustainable development[J]. ChemSusChem, 2016, 9(24): 3374-3381.
2	LACY F, KAILASAM M T, O'CONNOR D T, et al. Plasma hydrogen peroxide production in human essential hypertension: role of heredity, gender, and ethnicity[J]. Hypertension, 2000, 36(5): 878-884.
3	NUGRAHA M, TSAI M C, SU W N, et al. Descriptor study by density functional theory analysis for the direct synthesis of hydrogen peroxide using palladium-gold and palladium-mercury alloy catalysts[J]. Mol. Syst. Des. Eng., 2018, 3(6): 896-907.
4	CHINTA S, LUNSFORD J H. A mechanistic study of H₂O₂ and H₂O formation from H₂ and O₂ catalyzed by palladium in an aqueous medium[J]. J. Catal., 2004, 225(1): 249–255.
5	LIU G, LIANG H, TIAN Y, et al. Direct synthesis of hydrogen peroxide over Pd nanoparticles embedded between HZSM-5 nanosheets layers[J]. Chinese Journal of Chemical Engineering, 2020, 28(10): 2577-2586.
6	FORD D C, NILEKAR A U, XU Y, et al. Partial and complete reduction of O₂ by hydrogen on transition metal surfaces[J]. Surf. Sci., 2010, 604(19/20): 1565-1575.
7	TIAN P F, OUYANG L K, XU X C, et al. Density functional theory study of direct synthesis of H₂O₂ from H₂ and O₂ on Pd(111), Pd(100), and Pd(110) surfaces[J]. Chin. J. Catal., 2013, 34(5): 1002-1012.
8	OUYANG L, TIAN P F, DA G J, et al. The origin of active sites for direct synthesis of H₂O₂ on Pd/TiO₂ catalysts: interfaces of Pd and PdO domains[J]. J. Catal., 2015, 321(5): 70-80.
9	NOMURA Y, ISHIHARA T, HATA Y, et al. Nanocolloidal Pd-Au as catalyst for the direct synthesis of hydrogen peroxide from H₂ and O₂[J]. ChemSusChem., 2008, 1(7): 619-621.
10	STERCHELE S, BIASI P, CENTOMO P, et al. Pd-Au and Pd-Pt catalysts for the direct synthesis of hydrogen peroxide in absence of selectivity enhancers[J]. Applied Catalysis A: General, 2013, 468: 160-174.
11	NTAINJUA E N, FREAKLEY S J, HUTCHINGS G J. Direct synthesis of hydrogen peroxide using ruthenium catalysts[J]. Top. Catal., 2012, 55(11/12/13): 718-722.
12	OTTO T, RAMALLO-LÓPEZ J M, GIOVANETTI L J, et al. Synthesis of stable monodisperse AuPd, AuPt, and PdPt bimetallic clusters encapsulated within LTA-zeolites[J]. J. Catal., 2016, 342: 125-137.
13	LI G, EDWARDS J, CARLEY A F, et al. Direct synthesis of hydrogen peroxide from H₂ and O₂ using zeolite-supported Au-Pd catalysts[J]. Catal. Today, 2007, 122(3/4): 361-364.
14	EDWARDS J K, HUTCHINGS G J. Palladium and gold-palladium catalysts for the direct synthesis of hydrogen peroxide[J]. Angew. Chem.: Int. Ed., 2008, 47(48): 9192-9198.
15	NUGRAHA M, TSAI M C, RICK J, et al. DFT study reveals geometric and electronic synergisms of palladium-mercury alloy catalyst used for hydrogen peroxide formation[J]. Applied Catalysis A: General, 2017, 547: 69-74.
16	EDWARDS J K, PRITCHARD J, LU L, et al. The direct synthesis of hydrogen peroxide using platinum-promoted gold-palladium catalysts[J]. Angew. Chem.: Int. Ed., 2014, 53(9): 2381-2384.
17	FREAKLEY S J, HE Q, HARRHY J H, et al. Palladium-tin catalysts for the direct synthesis of H₂O₂ with high selectivity[J]. Science, 2016, 351(6276): 965-968.
18	TIAN P F, XU X Y, AO C, et al. Direct and selective synthesis of hydrogen peroxide over palladium-tellurium catalysts at ambient pressure[J]. ChemSusChem, 2017, 10(17): 3342-3346.
19	PIZZUTILO E, FREAKLEY S J, CHEREVKO S, et al. Gold-palladium bimetallic catalyst stability: consequences for hydrogen peroxide selectivity[J]. ACS Catal., 2017, 7(9): 5699-5705.
20	LIANG H R, TIAN Y J, ZHANG B F, et al. Direct synthesis of hydrogen peroxide on Pd nanosheets with edge decorated by Au nanoparticles[J]. Green Chemical Engineering, 2020. DOI: 10.1016/J.gce. 2020.09.012.
21	SALAMA T M, ALI I O, HANAFY A I, et al. A novel synthesis of NaA zeolite encapsulated iron() Schiff base complex: photocatalytic oxidation of direct blue-1 dye with hydrogen peroxide[J]. Materials Chemistry and Physics, 2009, 113(1): 159-165.
22	EDWARDS J K, SOLSONA B, LANDON P, et al. Direct synthesis of hydrogen peroxide from H₂and O₂ using Au-Pd/Fe₂O₃ catalysts[J]. J. Mater. Chem., 2005, 15(43): 4595-4600.
23	LEE S, CHUNG Y M. An efficient Pd/C catalyst design based on sequential ligand exchange method for the direct synthesis of H₂O₂[J]. Mater. Lett., 2019, 234: 58-61.
24	ISHIHARA T, OHURA Y, YOSHIDA S, et al. Synthesis of hydrogen peroxide by direct oxidation of H₂ with O₂ on Au/SiO₂catalyst[J]. Applied Catalysis A: General, 2005, 291(1-2): 215-221.
25	FREAKLEY S J, LEWIS R J, MORGAN D J, et al. Direct synthesis of hydrogen peroxide using Au-Pd supported and ion-exchanged heteropolyacids precipitated with various metal ions[J]. Catal. Today, 2015, 248: 10-17.
26	LEI J J, SONG H T, WEI Y B, et al. A novel strategy to enhance hydrothermal stability of Pd-doped organosilica membrane for hydrogen separation[J]. Microporous and Mesoporous Materials, 2017, 253: 55-63.
27	GALLINA G, GARCIA-SERNA J, SALMI T O, et al. Bromide and acids: a comprehensive study on their role on the hydrogen peroxide direct synthesis[J]. Industrial & Engineering Chemistry Research, 2017, 56(45): 13367-13378.
28	WILSON N M, FLAHERTY D W. Mechanism for the direct synthesis of H₂O₂ on Pd clusters: heterolytic reaction pathways at the liquid-solid interface[J]. J. Am. Chem. Soc., 2016, 138(2): 574-586.
29	PARK S, JUNG J C, SEO J G, et al. Direct synthesis of hydrogen peroxide from hydrogen and oxygen over palladium catalysts supported on SO₃H-functionalized SiO₂ and TiO₂[J]. Catalysis Letters, 2009, 130(3/4): 604-607.
30	KIM J, CHUNG Y M, KANG S M, et al. Palladium nanocatalysts immobilized on functionalized resin for the direct synthesis of hydrogen peroxide from hydrogen and oxygen[J]. ACS Catal., 2012, 2(6): 1042-1048.
31	LEWIS R J, EDWARDS J K, FREAKLEY S J, et al. Solid acid additives as recoverable promoters for the direct synthesis of hydrogen peroxide[J]. Industrial & Engineering Chemistry Research, 2017, 56(45): 13287-13293.
32	RATCHANANUSORN W, GUDARZI D, TURUNEN I. Catalytic direct synthesis of hydrogen peroxide in a novel microstructured reactor[J]. Chemical Engineering and Processing: Process Intensification, 2014, 84: 24-30.
33	BLANCO-BRIEVA G, MONTIEL-ARGAIZ M, DESMEDT F, et al. Effect of the acidity of the groups of functionalized silicas on the direct synthesis of H₂O₂[J]. Top Catal., 2017, 60(15/16): 1151-1155.
34	LANDON P, COLLIER P J, CARLEY A F, et al. Direct synthesis of hydrogen peroxide from H₂ and O₂ using Pd and Au catalysts[J]. Phys. Chem. Chem. Phys., 2003, 5(9): 1917-1923.
35	LARI G M, PUÉRTOLAS B, SHAHROKHI M, et al. Hybrid palladium nanoparticles for direct hydrogen peroxide synthesis: The key role of the ligand[J]. Angew. Chem. Int. Ed., 2017, 56(7): 1775-1779.
36	SIERRA-SALAZAR A F, LI W S J, BATHFIELD M, et al. Hierarchically porous Pd/SiO₂ catalyst by combination of miniemulsion polymerisation and sol-gel method for the direct synthesis of H₂O₂[J]. Catal. Today, 2018, 306: 16-22.
37	EDWIN N N, PICCININI M, PRITCHARD J C A, et al. Effect of halide and acid additives on the direct synthesis of hydrogen peroxide using supported gold-palladium catalysts[J]. ChemSusChem, 2009, 2(6): 575-580.
38	CENTOMO P, MENEGHINI C, STERCHELE S, et al. EXAFS in situ: the effect of bromide on Pd during the catalytic direct synthesis of hydrogen peroxide[J]. Catal. Today, 2015, 248: 138-141.
39	MELADA S, RIODA R, MENEGAZZO F, et al. Direct synthesis of hydrogen peroxide on zirconia-supported catalysts under mild conditions[J]. J. Catal., 2006, 239(2): 422-430.
40	PARK S, KIM T J, CHUNG Y M, et al. Direct synthesis of hydrogen peroxide from hydrogen and oxygen over palladium catalyst supported on SO₃H-functionalized SBA-15[J]. Catalysis Letters, 2009, 130(3/4): 296-300.
41	KIM S, LEE D W, LEE K Y, et al. Effect of Pd particle size on the direct synthesis of hydrogen peroxide from hydrogen and oxygen over Pd core-porous SiO₂ shell catalysts[J]. Catalysis Letters, 2014, 144(5): 905-911.
42	LEE J W, KIM J K, KANG T H, et al. Direct synthesis of hydrogen peroxide from hydrogen and oxygen over palladium catalyst supported on heteropolyacid-containing ordered mesoporous carbon[J]. Catal. Today, 2017, 293: 49-55.
43	SEO M G, KIM S, JEONG H E, et al. A yolk-shell structured Pd@void@ZrO₂ catalyst for direct synthesis of hydrogen peroxide from hydrogen and oxygen[J]. J. Mol. Catal. A: Chem., 2016, 413: 1-6.
44	PARK S, SEO J G, JUNG J C, et al. Direct synthesis of hydrogen peroxide from hydrogen and oxygen over palladium catalysts supported on TiO₂-ZrO₂ mixed metal oxides[J]. Catalysis Communications, 2009, 10(13): 1762-1765.
45	TORRENTE-MURCIANO L, HE Q, HUTCHINGS G J, et al. Enhanced Au-Pd activity in the direct synthesis of hydrogen peroxide using nanostructured titanate nanotube supports[J]. ChemCatChem, 2014, 6(9): 2531-2534.
46	SEO M G, LEE D W, HAN S S, et al. Direct synthesis of hydrogen peroxide from hydrogen and oxygen over mesoporous silica-shell-coated, palladium-nanocrystal-grafted SiO₂ nanobeads[J]. ACS Catal., 2017, 7(4): 3039-3048.

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