高温热冲击制备用于催化反应的高熵合金纳米颗粒

doi:10.1016/S1872-2067(23)64428-6

催化学报 ›› 2023, Vol. 48: 66-89.DOI: 10.1016/S1872-2067(23)64428-6

高温热冲击制备用于催化反应的高熵合金纳米颗粒

刘炎昌^a, 田新龙^b, 韩业创^c^,^*(), 陈亚楠^a^,^*(), 胡文彬^a

^a天津大学材料科学与工程学院, 天津300072
^b海南大学化学工程与技术学院, 南海海洋资源利用国家重点实验室, 海南省精细化学重点实验室, 海南海口570228
^c厦门大学化学化工学院, 固体表面物理化学国家重点实验室, 中国福建能源材料科学与技术创新实验室(嘉庚创新实验室), 福建厦门361005

收稿日期:2022-12-03 接受日期:2023-02-28 出版日期:2023-05-18 发布日期:2023-04-20
通讯作者: * 电子信箱: yananchen@tju.edu.cn (陈亚楠), ychan93@xmu.edu.cn (韩业创).
基金资助:
国家自然科学基金(52171219);国家自然科学基金(91963113);中国博士后科学基金(2022M722646)

High-temperature shock synthesis of high-entropy-alloy nanoparticles for catalysis

Yanchang Liu^a, Xinlong Tian^b, Ye-Chuang Han^c^,^*(), Yanan Chen^a^,^*(), Wenbin Hu^a

^aSchool of Materials Science and Engineering, Tianjin University, Tianjin 300072, China
^bState Key Laboratory of Marine Resource Utilization in South China Sea, Hainan Provincial Key Laboratory of Fine Chemistry, School of Chemical Engineering and Technology, Hainan University, Haikou 570228, Hainan, China
^cState Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Xiamen University, Xiamen 361005, Fujian, China

Received:2022-12-03 Accepted:2023-02-28 Online:2023-05-18 Published:2023-04-20
Contact: * E-mail: yananchen@tju.edu.cn (Y. Chen), ychan93@xmu.edu.cn (Y.-C. Han).
About author:Ye-Chuang Han (Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province, Xiamen University). Dr. Ye-Chuang Han received his B.A. degree from Nanchang Hangkong University in 2015, and his M.S. degree from University of Science and Technology of China in 2018, and his Ph.D. degree from Xiamen University in 2022. Now, he is carrying out his postdoctoral research at Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM) and Xiamen University under the supervision of Prof. Zhong-Qun Tian. His research interests mainly focus on the synthetic methodology under non-equilibrium high temperature.
Yanan Chen is a Professor in School of Materials Science and Engineering, Tianjin University. He received his Bachelor's degree and joint Ph.D. degree from University of Science and Technology Beijing/University of Maryland in 2012 and 2017 respectively. He was an advanced innovative fellow at Tsinghua University before joining in Tianjin University. His research mainly focuses on nanomaterials, devices, and systems for advanced energy storage and conversion. His research interests include high-temperature shock (HTS), ultrafast nanomanufacturing, metastable high throughput synthesis, emerging energy storages Li-ion and beyond, catalysis, artificial intelligence and interdisciplinary. He has published more than 100 research papers on international famous journals, including Nat. Energy, Nat. Commun., Sci. Adv., JACS, PNAS, Adv. Mater., Mater. Today, Nano Lett., Adv. Energy Mater., ACS Nano and has been cited nearly 7000 times (including many ESI highly cited papers).
Supported by:
National Natural Science Foundation of China(52171219);National Natural Science Foundation of China(91963113);China Postdoctoral Science Foundation(2022M722646)

摘要/Abstract

摘要：

先进功能材料的研发与合成技术的进步密切相关, 因此合成过程中动力学和热力学参数的精准控制对于材料的制备至关重要. 传统的高温制造工艺(比如马弗炉、管式炉), 由于缓慢的升温和降温速率(0-1 K s^-1), 可以视为由热力学主导的、时刻处于平衡状态的加热过程, 由此制备的产物大多具有最低的吉布斯自由能和稳定的原子排列, 属于热力学产物. 为了打破缓慢升降温速率导致的热力学限制, 以动力学为主导的、具有超快升降温速率的高温热冲击(HTS)的合成方法在近年被广泛研究. 与传统的高温制造工艺不同, HTS在瞬间通过巨大的能量驱动, 可以在秒或毫秒的时间内达到3000 K的峰值温度, 具有超快的升降温速率(≥10⁵ K s^-1), 而且, 该方法制备的产物大多只在局部范围内有极小的吉布斯自由能, 并非最稳定的状态, 是热力学不稳定的产物. 这种动力学主导的特征, 使其在新型材料(比如常规方法无法获得的高熵成分、热力学亚稳相和表面富缺陷)的探索及可控制备中展现出巨大的优势.
在HTS合成所取得的重要进展中, 高熵合金(HEAs)纳米颗粒由于具有灵活的组成空间和高熵混合结构, 在多相催化反应中展现出较好的活性、选择性以及稳定性, 从而受到越来越广泛的关注. HEAs是由5种或5种以上元素以近摩尔比的形式获得多主元合金, 由于多种组分导致的高熵效应、晶格畸变效应、缓慢扩散效应和“鸡尾酒”效应, HEAs被认为是理想的催化剂, 但是由于传统方法制备的HEAs多为尺寸较大的大块合金, 具有较低的比表面积, 这极大地限制了其在催化领域的应用.
HTS超高的冷却速率可以抑制HEAs的粗化或者相分离, 从而制备得到纳米级别的HEAs, 有效解决了上述问题.
尽管近年来有很多关于HTS和HEAs的相关研究, 都未在本质上探讨HTS的相关机理. 基于此, 本文从能量-空间-时间的角度出发, 在根本上探讨了HTS的物理化学原理, 全面介绍了具有代表性的HTS技术(焦耳加热、激光加热、微波加热)的设备及机理, 总结了HTS制备催化剂相比于传统的热力学主导的近平衡加热方法的优越性, 旨在促进新兴的HTS技术进步; 同时介绍了HEAs的概念和特点, 总结了利用HTS技术制备HEAs及其衍生物的最新进展; 最后, 对HTS和HEAs的未来研究方向做了总结与展望. 综上, 本文旨在对推进HTS和HEAs的发展、整合二者的优势做出贡献.

关键词: 高温热冲击, 焦耳加热, 激光加热, 微波加热, 高熵合金, 纳米材料, 催化反应

Abstract:

Rational design and precise fabrication of advanced functional materials are intimately linked to the technological advances in synthetic methodologies. The high-temperature shock (HTS) method, which involves an ultrafast heating/cooling rate (>10⁵ K s^-1) and features kinetics-dominated characteristics in material synthesis, exhibits high superiority in exploring and controllable preparation of novel materials that are typically unobtainable, such as high-entropy composition, thermodynamically metastable phases, and defect-rich surfaces. Among these significant advances, high-entropy alloy (HEA) nanoparticles are particularly prominent in heterogeneous catalytic reactions with remarkable activity, selectivity, and stability owing to their flexible composition space and high-entropy mixing structure. In this review, the physicochemical principles of HTS are presented, and the equipment and mechanisms of representative HTS techniques (e.g., Joule heating, laser heating, microwave heating) are comprehensively introduced, with the aim of accelerating the development of burgeoning HTS techniques. The concept and features of HEAs are also briefly introduced, and recent progress in the synthesis of HEAs using the HTS techniques is reviewed to provide a focused view on the unique advantages of HTS synthesis for HEAs and the exploration of novel materials. Finally, conclusions and perspectives are also provided for future investigations of HTS and HEAs, which have great significance in guiding their development and integrating their strengths.

Key words: High-temperature shock, Joule heating, Laser heating, Microwave heating, High-entropy alloy, Nanomaterial, Catalysis reaction

刘炎昌, 田新龙, 韩业创, 陈亚楠, 胡文彬. 高温热冲击制备用于催化反应的高熵合金纳米颗粒[J]. 催化学报, 2023, 48: 66-89.

Yanchang Liu, Xinlong Tian, Ye-Chuang Han, Yanan Chen, Wenbin Hu. High-temperature shock synthesis of high-entropy-alloy nanoparticles for catalysis[J]. Chinese Journal of Catalysis, 2023, 48: 66-89.

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图/表 18

Fig. 1. (a) Temperature-time curve for traditional near-equilibrium heating. (b) Kinetic and thermodynamic products possess different total free energies. (c) Temperature variation during HTS treatment. (d) Timeline for the development of Joule heating and laser heating. (b) Reproduced with permission [5]. Copyright 2021, American Chemical Society. (d) Reproduced with permission [8]. Copyright 2016, The Authors. Reproduced with permission [23]. Copyright 2018, American Association for the Advancement of Science. Reproduced with permission [30]. Copyright 2022, Springer Nature. Reproduced with permission [31]. Copyright 2021, American Chemical Society. Reproduced with permission [107]. Copyright 2022, Springer Nature.

Fig. 2. (a) Number of papers on the topic of “high-entropy alloy” (data derived from Web of Science). (b) Mechanism of catalytic reactions. (c) Number and species of active sites in bulk HEAs, conventional alloy NPs, and HEA-NPs.

Fig. 3. Energy-space-time field and temperature variation rate of Joule heating, laser heating, microwave heating, and near-equilibrium heating. (a) Coupling of energy, space, and time to construct a power density that can achieve HTS. (b) Comparison of energy-space-time characteristics of various heating methods. (c) Comparison of temperature variation rate for various heating methods. Smaller space, less time, and more energy result in greater power density and higher temperature variation rate. (c) Reproduced with permission [44]. Copyright 2019, American Chemical Society. Reproduced with permission [9]. Copyright 2020, WILEY‐VCH. Reproduced with permission [45]. Copyright 2019, WILEY‐VCH. Reproduced with permission [46]. Copyright 2022, American Chemical Society.

Fig. 4. Equipment and mechanism of HTS. Schematics of the experimental setup for conducting Joule heating (a), laser heating (c), and microwave heating (e). Mechanisms of Joule heating (b), laser heating (d), and microwave heating (f). (a) Reproduced with permission [8]. Copyright 2016, The Authors. (c) Reproduced with permission [51]. Copyright 2019, The Authors. (d) Reproduced with permission [52]. Copyright 2022, American Association for the Advancement of Science. (e) Reproduced with permission [53]. Copyright 2020, Springer Nature. (f) Reproduced with permission [54]. Copyright 2019, Wiley‐VCH.

Table 1 Comparison of different heating methods.

Parameter	Joule heating	Laser heating	Microwave heating	Near-equilibrium heating
Heating/cooling rate	10³-10⁵ K s^-1	> 10⁵ K s^-1	10²-10⁴ K s^-1	0-1 K s^-1
Peak temperature	2-3 × 10³ K	2-3 × 10³ K	1-2 × 10³ K s^-1	10² K
Productivity per batch	mg~g	mg	mg~ several tens g	mg~ several hundreds g
Size	nm, uniform	nm, uniform	nm, uniform	nm to μm, easy to gather
Substrate applicability	high	high	low	high
Cost	low	high	medium	medium
Energy consumption	low	low	medium	high

Fig. 5. Comparison of different synthetic methods in terms of temperature, size, productivity per batch, substrate applicability, and energy density. (a) Joule heating; (b) laser heating; (c) microwave heating; (d) near-equilibrium heating.

Fig. 6. (a) Functional relationship between the mixing entropy and the number of elements in equimolar alloys. (b) Comparison of mixing entropy in conventional alloys. (c) Schematic of four core effects of HEAs: high entropy effect in thermodynamics, lattice distortion effect in structure, sluggish diffusion effect in kinetics, and cocktail effect in performance. (c) Reproduced with permission [74]. Copyright 2017, Elsevier.

Table 2 Summary of the various catalytic applications of HEAs.

Reaction	Catalyst	Performance	Stability	Electrolyte	Ref.
HER	NiCoFePtRh	27 mV @10 mA cm^-2	100% of the initial current density after 85 h	0.5 mol L^-1 H₂SO₄	[36]
	PtNiFeCoCu	11 mV @10 mA cm^-2	no obvious negative shift after 10000^th CV cycle	1 mol L^-1 KOH	[101]
	FeCoNiCu@Pt	13.7 mV @10 mA cm^-2	slight fluctuations during 100 h stability test	1 mol L^-1 KOH	[102]
	FeCoNiCuPtIr	21 mV @10 mA cm^-2	morphology and structure unchanged after 24 h work	1 mol L^-1 KOH	[103]
OER	CoFeNiMnMoPi	270 mV @10 mA cm^-2	good stability after 500 CV scans	1 mol L^-1 KOH	[104]
	RuNiMoCrFeO	219 mV @10 mA cm^-2	up to 100 h at 100 mA cm^-2	0.5 mol L^-1 H₂SO₄	[105]
	IrRuCoNiCu	166 mV @10 mA cm^-2	150 h at 1000 mA cm^-2 with negligible change	1 mol L^-1 KOH	[106]
	PtIrCuCrNi	176 mV @10 mA cm^-2	no obvious potential augmentation after 72 h	1 mol L^-1 KOH	[107]
ORR	(HfZrLaVCeTiNdGdYPd)O	0.85 V @E_1/2	maintained 86% of its initial current after 100 h	0.1 mol L^-1 KOH	[25]
	PtPdRhFeCoNi	0.85 V @E_1/2	exhibited excellent stability after 5000 cycles	0.1 mol L^-1 KOH	[52]
	PtPdFeCoNi	0.92 V @E_1/2	6 mV negative shifted after 50000 cycles of ADT	0.1 mol L^-1 HClO₄	[108]
	PtPdFeCoNi	0.85 V @E_1/2	decreased by 29% after operation for 15 h	1 mol L^-1 KOH	[109]
MOR	PtPdFeCoNi	oxidation peak at 0.856 V and higher mass current density of 951.6 mA mg_Pt^-1	the current density dropped only by 33% for HEA and 57% for Pt/C after 1500 s	0.1 mol L^-1 HClO₄ with 0.5 mol L^-1 CH₃OH	[108]
MOR	CuAuAgPtPd	intense peak at 0.8 V	steady-state after 0.8 V for 1000s, affording a current of 14.7 μA	0.5 mol L^-1 KNO₃ with CH₃OH	[110]
NH₃ oxidation	PtPdRhRuCe	~100% conversion and >99% nitrogen oxide selectivity	Over ~30 h	—	[23]
CO oxidation	Pd₁@ (CeZrHfTiLa)O_x	onset temperature at ~80 °C and complete CO oxidation at 170 °C	750 °C for 10 h; textural and structural properties remained unchanged	—	[111]
CO oxidation	PtNiMgCuZnCoO	100% conversion at 155 °C	no loss of catalytic activity at 135 °C even after 40 h	—	[112]

Table 2 Summary of the various catalytic applications of HEAs.

Reaction	Catalyst	Performance	Stability	Electrolyte	Ref.
HER	NiCoFePtRh	27 mV @10 mA cm^-2	100% of the initial current density after 85 h	0.5 mol L^-1 H₂SO₄	[36]
	PtNiFeCoCu	11 mV @10 mA cm^-2	no obvious negative shift after 10000^th CV cycle	1 mol L^-1 KOH	[101]
	FeCoNiCu@Pt	13.7 mV @10 mA cm^-2	slight fluctuations during 100 h stability test	1 mol L^-1 KOH	[102]
	FeCoNiCuPtIr	21 mV @10 mA cm^-2	morphology and structure unchanged after 24 h work	1 mol L^-1 KOH	[103]
OER	CoFeNiMnMoPi	270 mV @10 mA cm^-2	good stability after 500 CV scans	1 mol L^-1 KOH	[104]
	RuNiMoCrFeO	219 mV @10 mA cm^-2	up to 100 h at 100 mA cm^-2	0.5 mol L^-1 H₂SO₄	[105]
	IrRuCoNiCu	166 mV @10 mA cm^-2	150 h at 1000 mA cm^-2 with negligible change	1 mol L^-1 KOH	[106]
	PtIrCuCrNi	176 mV @10 mA cm^-2	no obvious potential augmentation after 72 h	1 mol L^-1 KOH	[107]
ORR	(HfZrLaVCeTiNdGdYPd)O	0.85 V @E_1/2	maintained 86% of its initial current after 100 h	0.1 mol L^-1 KOH	[25]
	PtPdRhFeCoNi	0.85 V @E_1/2	exhibited excellent stability after 5000 cycles	0.1 mol L^-1 KOH	[52]
	PtPdFeCoNi	0.92 V @E_1/2	6 mV negative shifted after 50000 cycles of ADT	0.1 mol L^-1 HClO₄	[108]
	PtPdFeCoNi	0.85 V @E_1/2	decreased by 29% after operation for 15 h	1 mol L^-1 KOH	[109]
MOR	PtPdFeCoNi	oxidation peak at 0.856 V and higher mass current density of 951.6 mA mg_Pt^-1	the current density dropped only by 33% for HEA and 57% for Pt/C after 1500 s	0.1 mol L^-1 HClO₄ with 0.5 mol L^-1 CH₃OH	[108]
MOR	CuAuAgPtPd	intense peak at 0.8 V	steady-state after 0.8 V for 1000s, affording a current of 14.7 μA	0.5 mol L^-1 KNO₃ with CH₃OH	[110]
NH₃ oxidation	PtPdRhRuCe	~100% conversion and >99% nitrogen oxide selectivity	Over ~30 h	—	[23]
CO oxidation	Pd₁@ (CeZrHfTiLa)O_x	onset temperature at ~80 °C and complete CO oxidation at 170 °C	750 °C for 10 h; textural and structural properties remained unchanged	—	[111]
CO oxidation	PtNiMgCuZnCoO	100% conversion at 155 °C	no loss of catalytic activity at 135 °C even after 40 h	—	[112]

Table 3 Summary of different synthesis methods and their advantages and disadvantages.

Synthesis method	Advantage	Disadvantage	High-entropy composition	Thermal treatment	Ref.
Joule heating	complex component without phase separation, general preparation strategy, low cost, rapid heating/cooling rate, and nanoscale particles.	reaction parameters vary; however, careful control is required.	PtPdRhRuCe	2000 K, 55 ms	[23]
			PtPdRhRuIrAuCuFe-CoNiCrMnWMoSn	1800 K, 50 ms	[24]
			CoNiRuRhIr	1500 K, 0.5 s	[34]
			PtPdAuFeCoNiCuSn	1100 K, 55 ms-5 min	[35]
			PtPdFeCoNi	2000 K, 0.5 s	[109]
			(MgFeCoNiZn)O	1273 K, 30 s	[73]
			(CrMnFeCoNi)S	1650 K, 55 ms	[27]
			(MoTaTiWZr)B	3000 K, 2 min	[154]
Laser heating	fastest heating/cooling rate, general preparation strategy, ultrafine and uniform particles.	high cost and high energy may damage the sample surface.	CoCrFeNiAl	2000 K, 100 ns	[31]
			PtPdRhFeCoNi	5 ns	[52]
			FeCoNiCuPtIr	~1550 K, 50-1000 ms	[103]
			PtIrCuCrNi	30 min	[107]
			CoCrFeNiMn	1273 K, 20 min	[126]
			CrCoFeNiMnMo	40 ns	[127]
Microwave heating	medium heating rate, flexible operability, and can be integrated into other methods.	the necessity of microwave absorber limits the applications.	CoCrFeNiMo	1223 K, 20 min	[28]
			PtPdFeCoNi	1850 K, 100 ms	[155]
			(MgCuNiCoZn)O	at 850 W and 2.45 GHz, 3 min	[156]
			AuPtPdCu	343 K, 10 s	[157]
Arc melting	mature technical route, significant production, and is currently the most used method.	high energy, time consumption, and high cost.	AlCoCrFeNi	873-1273 K, 0.5-5 h	[142]
			AlCoCrFeTiNi	300~1500 K	[33]
			AlMoNbTaTiZr	1673 K, 26 h	[89]
			AlMoNbSiTaTiVZr	973-1073 K, 0.5 h	[92]
			TiZrNbTa	1773 K, 5 h	[95]
			TiVCrZrNbMoHfTaW	1373 K, 10 h	[141]
Mechanical alloying and milling	easy-to-form solid solution with fine grain crystal	easy to be polluted in reaction, high energy consumption.	(NiMgCuZnCo)O	room temperature	[147]
			FeCoNiAlTi	> 40 h	[87]
			Pd1@(CeZrHfTiLa)O	1173 K	[111]
Magnetron sputtering deposition	easy-to-form uniform film structure.	high cost and small quantities.	MoNbTaVW	500 W, 30 min	[148]
Magnetron sputtering deposition	easy-to-form uniform film structure.	high cost and small quantities.	(MoNbTaVW)N	0.5 Pa, 20 sccm flow rate	[149]
Fast-moving bed pyrolysis	simple equipment and easy operation.	different conditions in precursor reduction.	MnCoNiCuRhPdSnIrPtAu	923 K, 5 s	[121]
Fast-moving bed pyrolysis	simple equipment and easy operation.	different conditions in precursor reduction.	FeCoNiCuPdIrPtAu	923 K, 2 h	[151]
Aerosol synthesis	nanoscale uniform particles.	unsatisfactory generalization.	NiCoCuFePt	1372 K, 3 s	[152]
			CoFeNiMnMoPi	1173 K	[104]
			PdRuFeNiCuIr	2000 K, tens of milliseconds	[153]

Table 3 Summary of different synthesis methods and their advantages and disadvantages.

Synthesis method	Advantage	Disadvantage	High-entropy composition	Thermal treatment	Ref.
Joule heating	complex component without phase separation, general preparation strategy, low cost, rapid heating/cooling rate, and nanoscale particles.	reaction parameters vary; however, careful control is required.	PtPdRhRuCe	2000 K, 55 ms	[23]
			PtPdRhRuIrAuCuFe-CoNiCrMnWMoSn	1800 K, 50 ms	[24]
			CoNiRuRhIr	1500 K, 0.5 s	[34]
			PtPdAuFeCoNiCuSn	1100 K, 55 ms-5 min	[35]
			PtPdFeCoNi	2000 K, 0.5 s	[109]
			(MgFeCoNiZn)O	1273 K, 30 s	[73]
			(CrMnFeCoNi)S	1650 K, 55 ms	[27]
			(MoTaTiWZr)B	3000 K, 2 min	[154]
Laser heating	fastest heating/cooling rate, general preparation strategy, ultrafine and uniform particles.	high cost and high energy may damage the sample surface.	CoCrFeNiAl	2000 K, 100 ns	[31]
			PtPdRhFeCoNi	5 ns	[52]
			FeCoNiCuPtIr	~1550 K, 50-1000 ms	[103]
			PtIrCuCrNi	30 min	[107]
			CoCrFeNiMn	1273 K, 20 min	[126]
			CrCoFeNiMnMo	40 ns	[127]
Microwave heating	medium heating rate, flexible operability, and can be integrated into other methods.	the necessity of microwave absorber limits the applications.	CoCrFeNiMo	1223 K, 20 min	[28]
			PtPdFeCoNi	1850 K, 100 ms	[155]
			(MgCuNiCoZn)O	at 850 W and 2.45 GHz, 3 min	[156]
			AuPtPdCu	343 K, 10 s	[157]
Arc melting	mature technical route, significant production, and is currently the most used method.	high energy, time consumption, and high cost.	AlCoCrFeNi	873-1273 K, 0.5-5 h	[142]
			AlCoCrFeTiNi	300~1500 K	[33]
			AlMoNbTaTiZr	1673 K, 26 h	[89]
			AlMoNbSiTaTiVZr	973-1073 K, 0.5 h	[92]
			TiZrNbTa	1773 K, 5 h	[95]
			TiVCrZrNbMoHfTaW	1373 K, 10 h	[141]
Mechanical alloying and milling	easy-to-form solid solution with fine grain crystal	easy to be polluted in reaction, high energy consumption.	(NiMgCuZnCo)O	room temperature	[147]
			FeCoNiAlTi	> 40 h	[87]
			Pd1@(CeZrHfTiLa)O	1173 K	[111]
Magnetron sputtering deposition	easy-to-form uniform film structure.	high cost and small quantities.	MoNbTaVW	500 W, 30 min	[148]
Magnetron sputtering deposition	easy-to-form uniform film structure.	high cost and small quantities.	(MoNbTaVW)N	0.5 Pa, 20 sccm flow rate	[149]
Fast-moving bed pyrolysis	simple equipment and easy operation.	different conditions in precursor reduction.	MnCoNiCuRhPdSnIrPtAu	923 K, 5 s	[121]
Fast-moving bed pyrolysis	simple equipment and easy operation.	different conditions in precursor reduction.	FeCoNiCuPdIrPtAu	923 K, 2 h	[151]
Aerosol synthesis	nanoscale uniform particles.	unsatisfactory generalization.	NiCoCuFePt	1372 K, 3 s	[152]
			CoFeNiMnMoPi	1173 K	[104]
			PdRuFeNiCuIr	2000 K, tens of milliseconds	[153]

Fig. 7. (a) Illustration of the two approaches to perform rapid heating: thermal shock and fast-moving bed. (b) Kinetics dominate the formation of metallic glass, HEAs, and phase-separated structures. (c) New strategies based on high-temperature and high-entropy enable more alloy choices, such as high-entropy design to overcome the immiscibility of Au-X combinations. (d) Elemental maps of HEA-NPs composed of 15 different elements. (e) Schematic of roll-to-toll manufacturing of NPs. (f) Schematic of the HEA-NPs synthesis via an aerosol droplet-mediated technique thermal-treated with Joule heating; Schematic of the high-throughput synthesis of HEA-NPs (g) and fast screening of NPs for catalytic ORR (h). (i) Schematic for the preparation of HEAs@Pt. (a) Reproduced with permission [19]. Copyright 2022, Wiley‐VCH. Reproduced with permission [158]. Copyright 2019, Royal Society of Chemistry. (b) Reproduced with permission [23]. Copyright 2018, American Association for the Advancement of Science. (c) And (d) reproduced with permission [24]. Copyright 2021, Elsevier. (e) Reproduced with permission [158]. Copyright 2019, Royal Society of Chemistry. (f) Reproduced with permission [152]. Copyright 2020, American Chemical Society. (g) and (h) reproduced with permission [109]. Copyright 2020, The Authors. (i) Reproduced with permission [102]. Copyright 2022, The Authors.

Fig. 8. (a) Reaction scheme for ammonia oxidation as well as the structure and performance of HEA-NPs and multimetallic nanoparticles (MMNPs). (b,c) Catalytic performance of PtPdRhRuCe HEA-NPs; 4D-STEM and the selected pattern (d) and strain map (e) of the 15-HEA NPs. CV (f), LSV (g), and stability test (h) of PtPdFeCoNi HEA-NPs. Overpotential (i) and stability test (j) of HEA@Pt. (a-c) Reproduced with permission [23]. Copyright 2018, American Association for the Advancement of Science. (d) and (e) Reproduced with permission [24]. Copyright 2021, Elsevier. (f-h) Reproduced with permission [109]. Copyright 2020, The Authors. (i) and (j) Reproduced with permission [102]. Copyright 2022, The Authors.

Fig. 9. (a) Schematic of the fabrication of HEA-NPs by laser scanning ablation in liquids. (b) Schematic diagram of pulsed laser irradiation manufacturing in mixed salt solutions. (c) The four steps of the laser-induced thermionic emission reduction process for the synthesis of HEA-NPs on carbonaceous supports. (d) The curve of temperature-time during irradiation and the pictures of the laser heating process. (e) Corresponding EDX element mapping images, scale bar is 10 nm. (a) Reproduced with permission [107]. Copyright 2022, Springer Nature. (b) Reproduced with permission [31]. Copyright 2021, American Chemical Society. (c) Reproduced with permission [52] Copyright 2022, American Association for the Advancement of Science. (d) and (e) Reproduced with permission [103]. Copyright 2022, Wiley‐VCH.

Fig. 10. LSV curve of a two-electrode cell assembled by employing PtIrCoNiCr HEA as both cathode and anode for overall water splitting (a) and durability test at 200 mA cm-2 (b). CV curve (c) and stability measurement (d) of CoCrFeNiAl HECs. (e) ORR polarization plots of different HEA-NPs. (f) LSV plots of HER and OER for multi-element alloys. (g) Schematic illustrating the five most stable hollow sites for OH adsorption (red numbers) and five most unstable sites for H adsorption (black numbers). (h) Free-energy diagram of the OER of the hollow sites 1 and 5 for OH adsorption. (a) and (b) Reproduced with permission [107]. Copyright 2022, Springer Nature. (c) and (d) Reproduced with permission [31]. Copyright 2021, American Chemical Society. (e) Reproduced with permission [52] Copyright 2022, American Association for the Advancement of Science. (f-h) Reproduced with permission [103]. Copyright 2022, Wiley‐VCH.

Fig. 11. (a) Thermal treatment of the catalysts supported on carbon fiber cloth by microwave heating. (b) Schematic of microwave heating synthesis in a roll-to-roll process. (c) Schematic of the formation of HEA-NPs on rGO. (d) Temperature profile of the precursor treated by microwave heating. (I) and (II), before and during microwave heating, (III) the temperature color map and (Ⅳ) the corresponding uniform temperature distribution. XRD patterns of porous CoCrFeNiMo HEAs (e) and durability of HEAs catalyst for OER (f). Particle size (g), XRD (h), and EDX mapping (i) of AuPtPdCu HEA-NPs. (a) and (b) Reproduced with permission [171]. Copyright 2021, Wiley‐VCH. (c) and (d) Reproduced with permission [155]. Copyright 2021, American Chemical Society. (e) and (f) Reproduced with permission [28]. Copyright 2021, Elsevier. (g), (h) and (i) Reproduced with permission [157]. Copyright 2021, Springer Nature.

Fig. 12. Electrocatalytic performance of HEA-NPs. LSV curves (a), comparisons of overpotentials (b), and stability test (c) of PtRhCoNiCu/CC for HER. LSV curves (d), comparisons of overpotentials (e), and stability test (f) of IrRuCoNiCu/CC for OER. LSV curves (g) and chronopotentiometric curves (h) for water-splitting reaction. Reproduced with permission [106]. Copyright 2022, FJIRSM CAS, Fuzhou.

Fig. 13. (a) Synthesis of single-phase MEO-NPs based on temperature-driven, oxidation driven, and entropy-driven strategies. (b) The low-entropy catalysts prepared by near-equilibrium heating suffer from detachment and agglomeration, whereas the HTS high-entropy catalysts maintain good stability. (c) Schematics of the preparation of high entropy borides and the Joule heating method fills the temperature gap between the conventional furnace and arc melting methods. Schematics demonstrating the fabrication and structure (d), and particle size (e) of the HES-NPs. LSV curves (f) and schematic (g) of the constructed HES-NPs model by considering cationic Co centers as active sites. (h) OER and ORR LSV curves of HEMG-NPs ((CrCoFeNi)x is not marked). (a) Reproduced with permission [159]. Copyright 2021, Springer Nature. (b) Reproduced with permission [25]. Copyright 2021, Wiley‐VCH. (c) Reproduced with permission [154]. Copyright 2022, American Association for the Advancement of Science. (d), (e), (f) and (g) Reproduced with permission [27]. Copyright 2020, Wiley‐VCH. (h) Reproduced with permission [127]. Copyright 2021, The Authors.

Fig. 14. CH4 conversion (a) and catalytic stability (b) of 10-MEO-PdO. LSV curves (c) and chemical stability (d) of 10-HEO-NPs. LSV curves (e) and OER stability test (f) of (MnFeCoNiZn)O. (g) Two-dimensional map of the calculated overpotentials at Fe, Co, and Ni sites by DFT simulation. LSV polarization curves (h) and chronopotentiometric curves (i) of RuNiMoCrFeOx. (a) and (b) Reproduced with permission [159]. Copyright 2021, Springer Nature. (c) and (d) Reproduced with permission [25]. Copyright 2021, Wiley‐VCH. (e-g) Reproduced with permission [73]. Copyright 2022, American Chemical Society. (h) and (i) Reproduced with permission [105]. Copyright 2022, The Royal Society of Chemistry.

Fig. 15. Schematic of the perspectives for HTS and HEAs.

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高温热冲击制备用于催化反应的高熵合金纳米颗粒

High-temperature shock synthesis of high-entropy-alloy nanoparticles for catalysis

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