Review of MXenes as electrocatalysts for hydrogen production
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摘要: 基于可再生能源的电解水技术是生产“绿氢”的主要方法但受限于高电耗以及由此产生的高电力成本，电解水技术在大规模推广应用方面仍面临困难。降低电耗的途径在于开发高性能的电催化剂。MXenes是一种碳化物、氮化物和碳氮化物组成的二维材料，具有高导电性、大比表面积、高机械强度和优异的亲水性，是电催化剂的理想载体，被广泛应用于电解水制氢领域的研究。首先介绍了MXenes的基本组成与结构特征，其次总结分析了MXenes直接用于电解水制氢方面的研究成果，并阐述了其作为载体材料锚定高活性物质用于析氢和析氧反应的应用和进展，最后总结并展望了MXenes材料未来的发展前景。Abstract: Renewable energy-based water electrolysis is the main method of producing “green hydrogen”, but it still faces difficulties in large-scale application due to high power consumption and the resulting high cost of electricity. The way to reduce power consumption lies in the development of high-performance electrocatalysts. MXenes is a two-dimensional material composed of carbides, nitrides and carbon-nitrides with high electrical conductivity, large specific surface area, high mechanical strength and excellent hydrophilicity, which is an ideal carrier for electrocatalysts and has been widely used in the research in the field of hydrogen production by electrolysis of water. This paper firstly introduces the basic composition and structural characteristics of MXenes, summarizes and analyzes the research results on the direct use of MXenes in electrolysis of water for hydrogen production, and describes the application and progress of its use as a carrier material to anchor highly active substances for hydrogen and oxygen evolution reaction, and finally summarizes and looks forward to the future development prospects of MXenes materials.
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Key words:
- MXenes /
- electrochemical water splitting /
- carrier /
- application
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图 4 不同官能团MXenes的表征与理论计算
(a) Ti3C2Tx纳米片F 1s的XPS光谱[34]； Ti3C2Tx、Ti3C2(OH)x与Ti3C2Ox的XPS光谱：(b)F 1s与(c) O 1s[35]；Ti3C2Cl2与Ti3C2Tx的(d)拉曼光谱与(e)傅里叶红外光谱[37]； (f) Ta2CS2与Ta4C3Tx在Ta 4f的XPS光谱[39]；(g)不同官能团的归一化结合能与(h)相应的分布[40]
Figure 4. Characterization and theoretical calculations of MXenes with different functional groups
图 6 MXenes与贵金属化合物的形成、性能与理论计算
(a) Ru-RuO2/Ti3C2Tx催化剂的合成示意[47]； (b) Ti3C2Tx、Ru-RuO2/Ti3C2Tx与水的接触角测试[47]； (c) Ti3C2Tx与不同Ru负载量下Ru-RuO2/Ti3C2Tx的HER极化曲线[47]； (d) Ru-Ru2P/Ti3C2Tx催化剂的合成示意与其在AEMWE的应用[48]；(e) Ru-Ru2P与Ru-Ru2P/Ti3C2Tx催化剂Ru 3d轨道的投影态密度(PDOS)[48]； (f) RuO2-Ti3C2/NF在10、50与100 mA/cm2电流密度下不同电解质中的HER与OER过电位[49]； (g)析氧反应(OER)中的吸附氧化机制(AEM)和晶格氧化机制(LOM)[50]；(h) RuO2与RuO2-Mo2TiC2Tx催化剂的投影态密度(PDOS)[50]
Figure 6. Formation, properties and theoretical calculations of MXenes and precious metal compounds
图 7 MXenes与过渡金属化合物的形成、表征与理论计算
(a) Ni2P/Ti3C2Tx/NF合成示意[51]； (b) N-MoS2/Ti3C2Tx、MoS2/Ti3C2Tx与MoS2的态密度(DOS)[52]；(c) N-MoS2/Ti3C2Tx与MoS2/Ti3C2Tx在S与N位点的氢吸附吉布斯自由能台阶图[52]； (d) FeCoNiMnBOx与FeCoNiMnBOx/Ti3C2Tx的TOF[53]； (e) NiCo-LDH/Ti3C2Tx/NF的SEM图[54]； (f) Co2P与MXenes界面产生的电荷密度差分(黄色代表电子积累，蓝色代表电子损失)[55]
Figure 7. Formation, characterization and theoretical calculations of MXenes and transition metal compounds
图 8 MXenes与单/双原子催化剂的表征与理论计算
(a) PtSA-Mo2TiC2Tx的HAADF-STEM放大图像及其相应的模拟图像[58]; (b) PtSA-Ti3C2Tx、最近报道的MXenes基与Pt基催化剂质量活性比较[59]; (c) Ir-2 NS-Ti3C2Tx、Ir箔和IrO2的EXAFS谱的傅里叶变换[60]; (d)不同F/O比下Ti2CTx的交换电流密度i0与∆GH的火山图[61]; 新描述符预测∆GH用于(e)Ti2CO2-STM与(f)Zr2CO2-STM[62]; (g) CoNi-Ti3C2Tx与Co-Ti3C2Tx的EXAFS谱的傅里叶变换[63]; (h) CoNi-Ti3C2Tx与Ni-Ti3C2Tx的EXAFS谱的傅里叶变换[63]; (h) Ru与Ni、Pd、Pt分别负载于Mo2Ti2C3O2时*OH迁移的动态能垒[64]
Figure 8. Characterization and theoretical calculations of MXenes and single/double atom catalysts
表 1 MXenes直接用于电解水催化性能的对比
Table 1. Comparison of catalytic properties of MXenes directly used for electrolysis of water
电催化剂 电解液 电解液浓度/（mol·L−1） 应用 过电位@10 mAcm−2/mV 塔菲尔斜率/（mV·dec−1） 参考
文献Ti3C2Tx KOH 1 HER 188 110 [25] Ti3C2Tx KOH 1 OER 330 91 [25] Ti3C2Tx nanofibers H2SO4 0.5 HER 169 97 [26] Ti2CTx H2SO4 0.5 HER 609 124 [27] Mo2CTx H2SO4 0.5 HER 283 82 [27] V4C3Tx H2SO4 0.5 HER >700 236 [28] Nb4C3Tx KOH 1 HER 398 122.2 [29] Ti2CFx H2SO4 0.5 HER 170 100 [34] Ti3C2(OH)x H2SO4 0.5 HER 217 88.5 [35] Ti3C2Ox H2SO4 0.5 HER 190 60.7 [35] Ti3C2Cl2 KOH 1 HER 259 92 [37] Ti3C2Cl2 KOH 1 OER 150 48 [37] Ta2CS2 KOH 1 HER 73 61.1 [42] Ta2CS2 KOH 1 OER 243 66.9 [42] N-Ti3C2Tx H2SO4 0.5 HER 198 92 [41] N-Ti2CTx H2SO4 0.5 HER 215 67 [42] P-Mo2CTx H2SO4 0.5 HER 186 [43] 
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表 2 MXenes作催化剂载体用于电解水催化性能的对比
Table 2. Comparison of catalytic performance of MXenes as catalyst carriers for water electrolysis
电催化剂 电解液 电解液浓度/（mol·L−1） 应用 过电位(@10 mAcm−2)/mV 塔菲尔斜率/(mV·dec−1) 参考文献 Ru-RuO2/Ti3C2Tx KOH 1 HER 43 52.1 [47] Ru-Ru2P/V2CTx H2SO4 0.5 HER 37 61.3 [48] Ru-Ru2P/V2CTx KOH 1 HER 21 31.4 [48] RuO2-Ti3C2/NF KOH 1 HER 20 45.8 [49] RuO2-Ti3C2/NF KOH+ NaCl 1+0.5 HER 35 45.8 [49] RuO2-Ti3C2/NF KOH+海水 1 HER 45 45.8 [49] RuO2-Mo2TiC2Tx H2SO4 0.5 OER 222 50.4 [50] Ni2P/Ti3C2Tx/NF KOH 1 HER 135 86.6 [51] N-MoS2/Ti3C2Tx KOH 1 HER 80 100 [52] FeCoNiMnBOx/Ti3C2Tx KOH 1 OER 268 39.8 [53] NiCo-LDH/Ti3C2Tx/NF KOH 1 HER 123 86.6 [54] Ti2VC2Tx@MOF-Co2P KOH 1 HER 114 93.1 [56] Ti2VC2Tx@MOF-Co2P KOH 1 OER 246 28.18 [55] PtSA-Mo2TiC2Tx H2SO4 0.5 HER 30 30 [58] PtSA- Ti3C2Tx H2SO4 0.5 HER 38 45 [59] Ir-2NS-Ti3C2Tx H2SO4 0.5 HER 57.7 25.1 [60] Ir-2NS-Ti3C2Tx KOH 1 HER 40.9 50.5 [60] CoNi-Ti3C2Tx KOH 1 HER 31 33.0 [63] CoNi-Ti3C2Tx KOH 1 OER 241 79.8 [63]
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