2D-hBN：新兴的二维材料，特性和应用探索

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"这篇研究论文深入探讨了二维六方氮化硼（2D-hBN）的合成、性质及其在各种应用中的潜力。2D-hBN因其独特的光学、电学、机械、热稳定性和化学惰性特性，成为研究的焦点。它在场效应晶体管（FETs）、隧道器件、深紫外发射器和探测器、光电器件以及纳米填充材料等领域具有广泛应用。通过掺杂、替代和功能化等策略，可以调控2D-hBN的属性和功能，使其成为与石墨烯和过渡金属二硫属化物（TMDCs）等其他二维材料集成的关键材料，有望推动下一代微电子和其他技术的发展。" 本文详细介绍了二维六方氮化硼这一二维材料的重要特性。2D-hBN是一种与石墨烯结构相似的层状材料，但具有独特的性能。其光学和电学特性使它在电子器件中具有广泛的应用前景。例如，在场效应晶体管（FETs）中，2D-hBN的绝缘特性可以作为优良的栅极绝缘层，提高器件的性能。同时，由于其良好的热稳定性，2D-hBN也适用于高功率和高速电子设备，有助于散热。此外，2D-hBN的机械强度和化学惰性使得它在极端环境下的稳定性显著，这对于开发耐恶劣环境的电子设备至关重要。在深紫外发射器和探测器中，2D-hBN的宽禁带特性使其能够工作在短波长紫外光谱范围内，这对紫外光电子学领域有重大意义。在光电器件方面，2D-hBN的光响应性和光电转换能力使其成为潜在的光探测和光电转换材料。其纳米填充材料的角色则可能提升复合材料的性能，例如增强材料的导热性或电性能。论文还指出，通过掺杂和替代方法可以改变2D-hBN的性质，如改变其带隙或引入特定功能基团，以适应不同的应用需求。这种可调控性是2D-hBN在与其他二维材料（如石墨烯和TMDCs）集成时的一大优势，可以实现器件性能的优化和新功能的开发，为构建复杂的二维异质结构提供了可能性。 2D-hBN作为二维材料家族的重要成员，其优异的物理和化学特性使其在微电子、光电子和纳米技术等领域展现出巨大的应用潜力。通过深入研究和精细调控，2D-hBN有望推动科技领域的革新，并成为未来技术发展的重要基石。

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The Royal Society of Chemistry 2017 J. Mater. Chem. C, 2017, 5, 11992--12022 | 11997

of monolayer BN on metal substrates was reported in 1990, in

which BN was grown on Pt(111) and Ru(001) substrates by

adsorption and decomposition of borazine.

A 1 : 1 stoichio-

metry of B:N in borazine averts the complex deposition chemistry.

Diﬀerent eﬀective coverage ratios of monolayer BN were observed

at 0.36 and 0.15 for Pt(111) and Ru(001), respectively, due to the

diﬀerent degrees of dissociation on both substrates.

Oshima et al.

prepared single-crystalline monolayer hBN

on the Ni(111) substrate with borazine as the precursor. Similar

to what was observed by Paine,

the growth of the second or

more layers is pretty diﬃcult, and needs a precursor exposure

of B300 times higher than for the first layer formation. In

addition, the growth behavior and electronic properties of

monolayer hBN were almost independent of diﬀerences in

supporting substrates.

But the small diﬀerence in the lattice

constant between Ni(111) surface (2.49 Å) and bulk hBN (2.5 Å)

renders the Ni foil a promising substrate for 2D-hBN growth.

The elemental ratio of B and N, and the toxicity and liquid state

(melting point of B58 1C) of borazine at room temperature

make the experiment complicated. Alternatively, a more stable

and easy-to-handle precursor, B-trichloroborazine (ClBNH)

was investigated to substitute borazine for monolayer hBN

growth on Ni(111)

and Pt(111).

Both A-type (orientation of

the B and N sublattices coincides with the Pt(111) substrate)

and B-type (orientation of B and N sublattices rotated 301 versus

Pt(111) substrate) were observed in the monolayer hBN/Pt(111)

system. This demonstrated the significant influence of precursor

chemistry and substrate metals on the formation, orientation and

electronic structure of monolayer hBN. Some of these experiments

were designed to verify the electronic and optical properties

calculated.

In 2004, Corso et al.

synthesized hBN nanosheets in the

form of so-called nanomesh on a Rh(111) substrate (Fig. 3a and

b), which exhibit a high degree of periodicity. According to their

investigations of the crystal structure,

65–71

the pore shape and

size in the nanomesh are highly dependent on the type of

substrate used. Different from previous studies, a nanomesh

could be grown on Rh(111) and Ru(0001), while a flat mono-

layer hBN is formed when using Pd(111), Pt(111), Cu(111),

Mo(110), Cr(110), Fe(110), and Ni(111) as the substrate

(Fig. 3c). This was considered to relate to the different peculiarities

of the interfacial chemical bonding and the adsorption/decom-

position processes of precursors during the growth process on

these substrates. In particular, monolayer and nanomesh hBN

coexisted when synthesis was conducted on Ir(111). Four concrete

steps, (a) adsorption of borazine onto the substrate surface,

(b) decomposition of the precursor to form mobile surface

species, (c) diffusion and coalescence of species to form hBN

islands, (d) connection of hBN islands to form a compact hBN

nanomesh structure, were proposed on the basis of the real-time

microscopy conducted to study the formation of hBN nanomesh

on Rh(111),

Ru(0001),

and Ir(111),

in which temperature,

substrate conditioning, precursor type and concentration, and

partial pressure could all play a role.

It should be noted that a great advance had been made more

recently with the growth of hBN on a wafer scale. Monolayer hBN

was formed on a 4-inch Rh(111) substrate in a modified ultrahigh

vacuum chamber with a self-terminating process.

Corrugated

morphologies were observed with the hBN surface due to the

folded geometry of the Rh substrate. Similarly, wrinkling patterns

were also detected on epitaxial 2-inch hBN layers, which became

more serious with increasing thickness.

However, with a

modified low-pressure CVD method, few-layer wrinkle-free

hBN was reported uniformly grown on a 2-inch c-plane sapphire

substrate with AA

stacking order.

These new breakthroughs

provide possibilities for further investigation on the diverse

properties of hBN nanosheets and the applications of nanometer-

scale hBN in micro- and nanofabrication fields. Besides, epitaxial

strategies including van der Waals epitaxy (vdW-E),

77–79

molecular

beam epitaxy (MBE),

80,81

and atomic layer epitaxy (ALE)

have also

been explored to prepare hBN nanosheets, and the details are

summarized in Table 1, where the overall quality of the as-grown

hBN varies from one case to another, and the processing parameters

need to be optimized, especially for the catalyst substrates and

transfer technique.

2.3.2 CVD synthesis of hBN nanosheets on polycrystalline

or amorphous substrates. Although the epitaxy-based approaches

could produce monolayer hBN with generally high crystallinity,

they are in general extremely sensitive to the substrates, and most

of them are with specific orientations that need highly restricted

Fig. 3 (a and b) Constant-current STM images of the hBN nanomesh

formed on a Rh(111) surface. (a) Two steps on the Rh(111) surface are

shown. The black features are defects in the mesh, one of which is shown

with diﬀerent contrast in the inset. (b) Two layers of the hBN nanomesh are

shown by a high-resolution image which cover the Rh(111) surface. The

mesh unit cell is indicated. The cross-sectional profile along the diagonal

white line indicates four diﬀerent height levels. Reproduced with permission

overlayers on Pt(111), Ir(111), Rh(111), and Ru(0001) taken with hn =470eV

in normal emission, with the results of the corresponding peak-fit analysis.

Insets: Schematic representation of the h-BN morphology on diﬀerent

Elsevier Ltd.

Review Journal of Materials Chemistry C

11998 | J. Mater. Chem. C, 2017, 5, 11992--12022 This journal is

The Royal Society of Chemistry 2017

pretreatments, making most of them rather complicated and

time-consuming, and therefore diﬃcult for integration into large

scale practical manufacturing. Therefore, new facile strategies

need to be developed especially in order to synthesize large-area

and high-quality 2D-hBN on common substrates to meet the

general demands and preferably be compatible with silicon-based

processes. Generally speaking, any synthesis procedure can be

optimized, in order to control the lateral size, layer numbers,

and crystalline structure, making the fabrication process more

compatible and maneuverable for specific applications. As

catalyst-type substrates, Cu and Ni foils are traditionally used

for graphene and 2D-hBN growth, due to their low-cost and

excellent catalytic performance.

83,84

For convenience, some typical CVD processes for hBN

nanosheet growth are summarized, which employed borazine

and ammonia borane (borazane) with Cu,

85–91

Ni,

92,93

and

29,94–96

as substrates, as shown in Table 2. Annealing at high

temperature makes the substrates recrystallize with larger grain

size, which guarantees the coverage of synthesized hBN to range

from tens of microns to several centimeters. The morphology

and nucleation density are highly dependent on the pretreatment

of the substrates and decomposition of the precursors. In this

connection, studies that are focused on the optimization of various

process parameters have been performed. The type and initial

precursor input rate, precursor purity, and background pressure

are critical for the successful growth of atomic hBN layers.

97,98

expected, the nucleation density decreases with a decrease in the

flow rate, and the lateral growth can continue until coalescence

with another domain, and vice versa. Due to the incomplete

thermolysis and incorporation of certain doping atoms arising

from the contamination of precursors, high-quality and uniformly

thin hBN nanosheets are more inclined to be formed at low

pressure with pure precursors. Especially, with the observation

of a dominant crystal orientation, monolayer hBN was fabricated

on the melting Cu foil on a supporting W foil with B75% grain

alignment and full coverage, which provides an extensive study

on the aligned growth of hBN single crystals over large areas.

A strong alignment of hBN leads to their convergence to

symmetrical multifaceted shapes (such as ‘‘butterfly’’ and

‘‘6-apex-star’’).

In addition to the common substrates, other catalyst-based

substrates were also explored. For example, uniform monolayer

hBN could be synthesized on a heteroepitaxial Co film,

but

the incomplete coverage is a major problem. By choosing the

Cu–Ni alloy as the substrate, Lu et al.

developed single-crystal

monolayer hBN grains with areas up to 7500 mm,

which is

about two orders larger than those reported previously. The

introduction of Ni could effectively reduce the nucleation

density to 60 per mm

, thus giving rise to large sizes of hBN

nanosheets (Fig. 4a–c). Likewise, an active Si-doped Fe sub-

strate could be applied to effectively tune the nucleation density

of hBN via controlling the amount of Si diffusion into the Fe

thin film.

100

However, the grain boundary between two hBN

domains seriously impacts the quality of the as-grown nanosheets

in spite of the controllability of nucleation density and even on

layer number. Based on this consideration, Kim et al.

101

devised a

promising strategy for wafer-scale and defect-free hBN fabrication,

where nanocrystalline graphene (nc-G) acted as a seed layer for the

growth of the large-area hBN (Fig. 4d and e).

To prevent chemical contamination during the transfer

process and make the process compatible with the CMOS

process, investigations into the growth of hBN on insulating

substrates, such as SiO

/Si, without catalyst and the subsequent

transfer process have been conducted. Yu et al.

reported a

catalyst-free method to grow hBN nanosheets on Si substrates

by microwave plasma CVD (MPCVD), where the triangular hBN

nanosheets thus obtained were ranging from 0.8 to 2.5 mmin

size with diﬀerent tilting angles to substrates. Also, a mixture of

Table 1 The deta ils of other epitaxial strategies for the synthesis of hBN

Ref. Method Substrate Growth parameters Conclusions

77 vdW-E Graphene 900 1C

Borazine

10–100 Pa

Few-layer hBN preferred to grow on graphene than on SiO

/Si with

triangular morphology on narrow graphene belts, but with polygonal

morphology on large graphene films

78 vdW-E Cu(111) foil 1000 1C

Ammonia borane

The triangular monolayer hBN was synthesized in a low-pressure system

and it continued to coalesce to a thin film with increasing growth time

79 vdW-E Cu(102) and

Cu(103) foils

1035 1C

Ammonia borane

0.1 Pa

Triangular monolayer hBN was achieved with diﬀerent unidirectional

aligned growth on diﬀerent faceted Cu foils

80 MBE Poly-crystalline

Ni foil

730–835 1C for growth, 1850 1C

for B atoms, and RF-350 W

for active N species

1.1  10

5

mbar

Highly crystalline hBN nanosheets were achieved with wrinkles and

ridges over the entire film. The initial ‘‘star’’-shaped islands evolved

into a closed film with increasing growth time

81 MBE Ni(111) foil 700 1C for growth, 1900 1C for

B atoms, and RF-250 W for

active N species 1.3  10

5

Torr

Multilayer hBN films were achieved with very high structural perfection

and AB stacking of BN layers. The elongated shape of the stripes

appeared, which might be attributed to the tough surface

82 ALE Co(0001) film 600 K

BCl

/NH

350 mTorr

Highly oriented hBN(0001) films were obtained with excellent uniformity,

continuity, and conformality on the macroscopic scale. The thickness

is controllable, which is proportional to the number of BCl

/NH

cycles

Journal of Materials Chemistry C Review

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