金属气凝胶：可控制备与应用展望

doi:10.3866/PKU.WHXB202212014

Abstract

Abstract:

Emerging as one of the youngest members in the family of porous materials, metal aerogels (MAs) are a new class of aerogels entirely built of nanostructured metals such as gold, silver, palladium, platinum, ruthenium, rhodium, osmium, copper, and nickel. They are typically fabricated via a sol-gel process coupled with special drying techniques (e.g., supercritical drying and freeze-drying). Combining the unique physicochemical properties of various nanostructured metals with the structural attributes of aerogels, MAs mark rapid mass transfer channels, highly conductive three-dimensional (3D) networks, and optical and magnetic properties. In this regard, MAs outperform conventional materials in various territories such as electrocatalysis, enzyme-like catalysis, surface-enhanced Raman scattering, diverse sensing, and actuators. Additionally, a substantial number of metal elements can offer vast opportunities for creating numerous MAs featuring desired properties, which is critical for a deep exploration and releases the full potential of aerogels. Consequently, MAs have received wide attention since their discovery in 2009.However, compared with conventional aerogels, MAs only appeared around a decade ago. A short research history challenges their fundamental studies, including controlled synthesis and structure-performance investigations, thereby retarding on-target materials design for practical applications. Currently, the majority of studies are restricted to MAs based on noble metals. This fact is ascribed to both their intrinsically high catalytic activity and simple fabrication due to the relatively high redox potential. In contrast, reports on low-cost non-noble metal aerogels are largely constrained, not to mention controlled synthesis as well as practical applications. As a result, the compositional and structural diversity of MAs is highly limited. Furthermore, the scope of the application of MAs is still constrained and is mostly restricted to electrocatalysis. Though certain remarkable MA-based electrocatalysts have been reported in the last few years, their limited composition and structure have retarded the systematic investigations into correlations between the material parameters and electrocatalytic properties. This discourages on-demand material design and performance optimization. Hence, fundamental studies and application attempts need to be strengthened to allow further development of this new material system. On this occasion, it is essential to thoroughly summarize the knowledge and design principles of MAs that have been presented in the past ten years. This study comprehensively introduces the state-of-the-art research progress in this field, which includes synthesis strategies, potential gelation mechanisms, and diverse applications of MAs. Additionally, the challenges and opportunities presented by MAs will be drawn from aspects of synthesis and applications. This review expects to attract widespread scientists from different fields (e.g., chemistry, physics, materials science, and life science) to join the area of MAs, thus jointly promoting the development of this young and promising field.

Key words: Aerogels, Metal, Sol-gel, Nanostructures, Electrocatalysis

Ning Wang, Yi Li, Qian Cui, Xiaoyue Sun, Yue Hu, Yunjun Luo, Ran Du. Metal Aerogels: Controlled Synthesis and Applications[J]. Acta Phys. -Chim. Sin. 2023, 39(9), 2212014. doi: 10.3866/PKU.WHXB202212014

Figures/Tables 21

Fig 1

Fig 2

Fig 3

Fig 4

Fig 5

Fig 6

Fig 7

Fig 8

Fig 9

Table 1

Summary of preparation methods and product parameters of typical MAs."

Composition	Initiating method or initiator	Gelation time	Density/(mg∙cm⁻³)	Ligament size/nm	Specific surface area/(m²∙g⁻¹)	Reference
Ag	evaporation concentration (313 K)	–	88	113	5.5	23
Au ^a	H₂O₂	~1 week	–	100–500	–	21
Ag ^a	H₂O₂	15 days	–	50–100	–	21
Pt ^a	ethanol	4 weeks	–	–	–	21
Ag ^a	C(NO₂)₄	4–12 h	37–41	5–11 ^b	43–160	45
Au-Ag-Pd ^a	C(NO₂)₄	16–24 h	20–60	4–6	76–269	47
Au-Ag	NaCl	1–28 days	70	15.4 ^b	42	58
Pd-Ag	NaCl	1–28 days	10	13.0 ^b	42	58
Pt-Ag	NaCl	1–28 days	180	13.6 ^b	32	58
Pd ^a	Ca²⁺	5 min–2 months	25–59	3–10	40–108	59
Au	NH₄F, NaCl, MgCl₂, KCl, NH₄NO₃, NH₄SCN, etc.	4–12 h	83.0–212.8	6.9–113.7	2.5–29.7	42
Ag	NH₄F	4–12 h	64.8	21.9	5.2	42
Pt	NH₄F	4–12 h	61.4	42	3.4	42
Pd	NH₄F	4–12 h	44.0–62.2	3.7	122.7	42
Au-M (M = Ag, Pd, Pt)	NH₄F	12 h		3.1–5.8	34.8–68.8	42
Pd-Pt	NH₄F	12 h		4.0	58.0	42
Au-Pd-Pt	NH₄F	12 h		3.8	95.8	42
Au	dopamine	6–72 h	40–43	5–6	50.1	48
Pd_xPt_y-Ni ^a	NaBH₄ (348 K)	＜6 h	35–50	4–8	67.7–95.4	68
Pd-Pt	NaBH₄	3–17 days	50–100	4–5	73–168	52
Au ^a	NaBH₄, DMAB, NaH₂PO₂	a few minutes	540	18–280	3.1	70
Pd ^a	NaBH₄, DMAB, NaH₂PO₂	a few minutes	65	12–65	15.4	70
Pt ^a	NaBH₄, DMAB, NaH₂PO₂	A few minutes	55	13–60	20.6	70
Pd ^a	CO (313 K)	5 h	11	50–100 ^c	–	73
Au	excessive NaBH₄	2–12 h	60.5–576.5	4.8–38.3	3.5–59.8	54
Ag, Pt, Os	excessive NaBH₄	4–6 h	157.2–250.6	48.2–226.7	2.1–13.2	54
Ru, Rh	excessive NaBH₄	4–6 h	–	3.9–2.5	1.2–3.8	54
Pd	excessive NaBH₄	4–6 h	51.8	5.6	69.1	54
Au-M (M = Ag, Pd, Pt, Ir)	excessive NaBH₄	4–6 h	46.7–169.8	4.3–7.6	42.6–72.9	54
Ni_xBi_y	excessive NaBH₄	8 h	–	30–36	12–44	34
Fe-Co-Ni	excessive NaBH₄	6 h	36	52.8	30.7	76
Pt ^a	N₂H₄ (hexane)	1–5 h	190–200	3–8	30–40	57
Cu NWs	N₂H₄ (323–358 K)	15 h	3.8–7.5	70–90	–	24
Ir_xCu	NaBH₄ (343 K)	2–3 h	–	3–7	41.7	77
Cu NWs	NaBH₄ (353 K)	~1 h	4.3–7.5	~130	–	75
Cu-Fe-Ni	DMAB (313K)	12 h	–	–	42	71
Pd	Na₂CO₃ (338 K)	~1 h	–	3–8	50.1	78
Au	freeze-casting	–	6–23	~7	–	79
Au ^a	freeze-casting	–	20–60	200–500	–	80
Ag ^a	freeze-casting	–		10–50	15	80
Pd ^a	freeze-casting	–		3–7	15	80
Pt ^a	freeze-casting	–		3–10	33	80
Cu NWs	freeze-casting	–	4.6–13.5	–	–	81
Au	freeze-thaw	12–24 h	164.4	35.0	–	82
Pd	freeze-thaw	12–24 h	–	4.5	–	82
Rh	freeze-thaw	12–24 h	–	4.8	–	82
Au-Pd	freeze-thaw	12–24 h	35.9 60.6	4.3	83.6 74.5	82
Au-Pt	freeze-thaw	12–24 h	35.9 60.6	4.7	83.6 74.5	82
Au	stirring	1–10 min	–	10.4–19.8	–	83
Ag	stirring	1–10 min	–	18.1	–	83
Rh	stirring	1–10 min	–	4.1	–	83
Pd	stirring	1–10 min	–	5.8	76.6	83
Au-M (M = Ag, Pd, Pt, Rh, Ir, Pd-Pt)	stirring	1–10 min	–	3.7–7.2	32.0–83.6	83
Ni NWs	N₂H₄ (353 K, magnetic field)	1 h	20–24	200–500	1.34–4.96	84
Pt-Ag_HCl	HCl (GRR)	8 h	–	7–10 ^b	24.7	85
Pt-Ag_NH4OH	NH₄OH (GRR)	8 h	–	7–10 ^b	83.4	85

Table 1

Fig 10

Fig 11

Fig 12

Fig 13

Fig 14

Table 2

Summary of the relevant parameters of MAs applied to alcohol oxidation reactions."

Composition	Electrolyte solution	Types of alcohol	I_f	Reference
AuPt₅	1 mol∙L⁻¹ H₂SO₄ + 1 mol∙L⁻¹ methanol	methanol	0.51 A∙mg_Pt⁻¹	87
Pt₄Ru₁Cu₅	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ methanol	methanol	2.1 A∙mg_Pt+Ru⁻¹	123
Ni₉₇Bi₃	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ methanol	methanol	1.8 A∙mg⁻¹	34
Pt-Cu	0.5 mol∙L⁻¹ H₂SO₄ + 1 mol∙L⁻¹ methanol	methanol	4.1 A∙mg_Pt⁻¹	74
Pt₁Cu₁Ir_0.04	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ methanol	methanol	4.7 A∙mg_Pt⁻¹	124
Pd	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ methanol	methanol	3.0 A∙mg_Pd⁻¹	98
Bi-decorated Pt	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ methanol	methanol	8.0 A∙mg_Pt⁻¹	125
Au_0.166Ag_0.288Pt_0.546	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ methanol	methanol	2.0 A∙mg_Pt⁻¹	126
Pt₃Cu₁	0.5 mol∙L⁻¹ H₂SO₄ + 1 mol∙L⁻¹ methanol	methanol	3.8 A∙mg_Pt⁻¹	127
Pd	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ ethanol	ethanol	8.8 A∙mg_Pd⁻¹	98
Pd_β-CD	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ ethanol	ethanol	7.8 A∙mg_Pd⁻¹	51
Pd₈₃Ni₁₇	1 mol∙L⁻¹ NaOH + 1 mol∙L⁻¹ ethanol	ethanol	3.6 A∙mg_Pd⁻¹	63
Pd₆₈Cu₃₂	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ ethanol	ethanol	3.5 A∙mg_Pd⁻¹	25
Ni-Pd₆₀Pt₄₀	1 mol∙L⁻¹ NaOH + 1 mol∙L⁻¹ ethanol	ethanol	6.9 A∙mg_Pd+Pt⁻¹	68
Pd	1 mol∙L⁻¹ NaOH + 1 mol∙L⁻¹ ethanol	ethanol	~3.2 A∙mg_Pd⁻¹	72
Pd	1 mol∙L⁻¹ KOH + 0.5 mol∙L⁻¹ ethanol	ethanol	4.7 A∙mg_Pd⁻¹	78
Au-Pd	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ ethanol	ethanol	2.7 A∙mg_Pd+Pt⁻¹	42
Au-Pd-Pt	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ ethanol	ethanol	4.8 A∙mg_Pd+Pt⁻¹	42
Pd-Ir	1 mol∙L⁻¹ KOH + 0.5 mol∙L⁻¹ ethanol	ethanol	5.4 A∙mg_Pd⁻¹	121
Au-Pd (PVP)	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ ethanol	ethanol	9.8 A∙mg_Pd⁻¹	53
Au	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ ethanol	ethanol	0.27 A∙mg⁻¹	92
Pt	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ ethanol	ethanol	0.99 A∙mg⁻¹	92
Pd	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ ethanol	ethanol	1.5 A∙mg⁻¹	92
Au₂Cu@Pd-₂	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ ethanol	ethanol	22.1 A∙mg_Pd⁻¹	96
Pd_89.3Au_10.7	1 mol∙L⁻¹ KOH + 0.5 mol∙L⁻¹ ethanol	ethanol	6.3 A∙mg_Pd⁻¹	122
Au-Pt	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ ethanol	ethanol	3.5 A∙mg_Pt⁻¹	82
Au-Pd	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ ethanol	ethanol	8.4 A∙mg_Pd⁻¹	82
Au-Pt	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ ethanol	ethanol	7.3 A∙mg_Pt⁻¹	83
Au-Pd-Pt	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ ethanol	ethanol	9.1 A∙mg_Pd+Pt⁻¹	83
Au-Pd-Pt with light	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ ethanol	ethanol	13.2 A∙mg_Pd+Pt⁻¹	83
Pd₃Pb₁@Pd	1 mol∙L⁻¹ KOH + 0.5 mol∙L⁻¹ glycol	glycol	6.4 A∙mg_Pd⁻¹	69
Pd	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ glycol	glycol	~7.8 A∙mg_Pd⁻¹	98
Pd	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ isopropanol	isopropanol	~1.7 A∙mg_Pd⁻¹	98
Pd	1 mol∙L⁻¹ KOH + 1 mol∙L⁻¹ glycerol	glycerol	~3.5 A∙mg_Pd⁻¹	98

Table 2

Fig 15

Fig 16

Fig 17

Fig 18

Fig 19

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