CIESC Journal ›› 2022, Vol. 73 ›› Issue (9): 3802-3814.DOI: 10.11949/0438-1157.20220327
• Reviews and monographs • Previous Articles Next Articles
Huihuang FANG(), Jinxing CHENG, Yu LUO(), Chongqi CHEN, Chen ZHOU, Lilong JIANG()
Received:
2022-03-02
Revised:
2022-07-28
Online:
2022-10-09
Published:
2022-09-05
Contact:
Yu LUO, Lilong JIANG
方辉煌(), 程金星, 罗宇(), 陈崇启, 周晨, 江莉龙()
通讯作者:
罗宇,江莉龙
作者简介:
方辉煌(1991—),男,博士,副研究员,hhfang@fzu.edu.cn
基金资助:
CLC Number:
Huihuang FANG, Jinxing CHENG, Yu LUO, Chongqi CHEN, Chen ZHOU, Lilong JIANG. Recent progress on ammonia oxidation catalysts at anode and their performances in low-temperature direct ammonia alkaline exchange membrane fuel cells[J]. CIESC Journal, 2022, 73(9): 3802-3814.
方辉煌, 程金星, 罗宇, 陈崇启, 周晨, 江莉龙. 氨电氧化催化剂及其低温直接氨碱性膜燃料电池性能的研究进展[J]. 化工学报, 2022, 73(9): 3802-3814.
反应中间物质 | 表征技术 | 文献 |
---|---|---|
N-3参与AOR反应 | SERS | [ |
N2H4、NO中间体;NO抑制了电化学反应 | ATR-IR | [ |
低电位区(E(vs SCE)<-0.50 V):N2H4、NH2 | FTIR | [ |
高电位区(E(vs SCE)>-0.10 V):N2O、NO2- | FTIR | [ |
NO、NO2、N2H4 | ATR-FTIR | [ |
N2、NO和N2O | DEMS | [ |
Table 1 The intermediates of AOR process by in situ characterization techniques
反应中间物质 | 表征技术 | 文献 |
---|---|---|
N-3参与AOR反应 | SERS | [ |
N2H4、NO中间体;NO抑制了电化学反应 | ATR-IR | [ |
低电位区(E(vs SCE)<-0.50 V):N2H4、NH2 | FTIR | [ |
高电位区(E(vs SCE)>-0.10 V):N2O、NO2- | FTIR | [ |
NO、NO2、N2H4 | ATR-FTIR | [ |
N2、NO和N2O | DEMS | [ |
催化剂 | 电解液溶液 | 扫描速率/ (mV·s-1) | 起始电位 (vs RHE)/V | 峰值电流密度 | 文献 |
---|---|---|---|---|---|
PtIr/CNT (Pt∶Ir=4∶1) | 0.1 mol·L-1 NH3 + 0.1 mol·L-1 KOH | 50 | 0.38 | 230 mA·cm-2 ECSA | [ |
PtIr/N-rGO (Pt∶Ir=1∶3) | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 10 | 约0.37 | 71 A·g-1 | [ |
PtRh/C (Pt∶Rh=9∶1) | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 20 | -0.44① | 93.8 A·g-1 | [ |
Pt/SiO2-CNT | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 5 | 0.484 | 77.3 A·g-1 | [ |
PtIr/C | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 5 | 0.43 | 25.1 A·g-1 | [ |
Pt5Ir5/SiO2-CNT | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 5 | 0.369 | 66.3 A·g-1 | [ |
PtIr/ SiO2-CNT (Pt∶Ir=9∶1) | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 5 | 0.42 | 90.6 A·g-1 | [ |
PtIrNi1/SiO2-CNT (Pt∶Ir=9∶1) | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 5 | 0.399 | 124 A·g-1 | [ |
PtZn | 0.1 mol·L-1 NH3 + 0.5 mol·L-1 KOH | 100 | 0.42 | 0.60 mA·cm-2 ECSA | [ |
PtIrZn (Pt∶Ir=8∶2) | 0.1 mol·L-1 NH3 + 0.5 mol·L-1 KOH | 100 | 0.30 | 0.56 mA·cm-2 ECSA | [ |
CuPtRu (Pt∶Ru=7∶1) | 1 mol·L-1 KOH saturated with NH3 | 20 | 0.49 | 180 A·g-1 | [ |
PtIrZn2/CeO2-ZIF-8 | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 5 | 0.35 | 31.8 A·g-1 | [ |
PtIrZn2/SiO2-CNT-COOH | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 5 | 0.35 | 61.4 A·g-1 | [ |
PtIr/SiO2-CNT-COOH | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 5 | 0.33 | 64.6 A·g-1 | [ |
PtIrCu HCOND | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 5 | 0.35 | 122.9 A·g-1 | [ |
PtNi | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 10 | 0.69 | 75 A·g-1 | [ |
PtAu/C (Pt∶Au=7∶3) | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 20 | 0.51 | 90 A·g-1 | [ |
PtNi | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 10 | 约0.5 | 75.32 A·g-1 | [ |
Pt/C | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 50 | 约0.52② | 39.9 A·g-1 | [ |
PtNi/C | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 50 | 约0.55② | 76.4 A·g-1 | [ |
PtNiO/C | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 50 | 约0.55② | 86.9 A·g-1 | [ |
Ni98Pd2 | 0.5 mol·L-1 NaNO3 + 0.2 mol·L-1 NH4NO3 | 50 | 1.3① | 150 A·g-1 | [ |
NiCu/C | 55 m mol·L-1 NH4Cl + 0.5 mol·L-1 NaOH | 25 | 0.47② | 52 mA·cm-2 | [ |
NiCu/C | 0.5 mol·L-1 NH3 + 1 mol·L-1 KOH | 50 | 0.4① | 110.4 mA·cm-2 | [ |
NiCu/C | 55 m mol·L-1 NH4Cl + 0.5 mol·L-1 NaOH | 25 | 0.43① | 105 mA·cm-2 | [ |
Ni(OH)2/C | 55 m mol·L-1 NH4Cl + 0.5 mol·L-1 NaOH | 25 | 0.43① | 15 mA·cm-2 | [ |
NiCr/C | 55 m mol·L-1 NH4Cl + 0.5 mol·L-1 NaOH | 25 | 0.40① | 10 mA·cm-2 | [ |
NiMn/C | 55 m mol·L-1 NH4Cl + 0.5 mol·L-1 NaOH | 25 | 0.40① | 20 mA·cm-2 | [ |
NiCo/C | 55 m mol·L-1 NH4Cl + 0.5 mol·L-1 NaOH | 25 | 0.35① | 10 mA·cm-2 | [ |
NiZn/C | 55 m mol·L-1 NH4Cl + 0.5 mol·L-1 NaOH | 25 | 0.45① | 2 mA·cm-2 | [ |
Ni(OH)2 on NiOOH | 0.1 mol·L-1 NaSO4 + 0.003 mol·L-1 NH3 | 10 | 0.6① | 2.7 mA·cm-2 | [ |
①vs Hg/HgO。 ②vs Ag/AgCl。 |
Table 2 Activity of AOR over non-/noble metallic catalysts
催化剂 | 电解液溶液 | 扫描速率/ (mV·s-1) | 起始电位 (vs RHE)/V | 峰值电流密度 | 文献 |
---|---|---|---|---|---|
PtIr/CNT (Pt∶Ir=4∶1) | 0.1 mol·L-1 NH3 + 0.1 mol·L-1 KOH | 50 | 0.38 | 230 mA·cm-2 ECSA | [ |
PtIr/N-rGO (Pt∶Ir=1∶3) | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 10 | 约0.37 | 71 A·g-1 | [ |
PtRh/C (Pt∶Rh=9∶1) | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 20 | -0.44① | 93.8 A·g-1 | [ |
Pt/SiO2-CNT | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 5 | 0.484 | 77.3 A·g-1 | [ |
PtIr/C | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 5 | 0.43 | 25.1 A·g-1 | [ |
Pt5Ir5/SiO2-CNT | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 5 | 0.369 | 66.3 A·g-1 | [ |
PtIr/ SiO2-CNT (Pt∶Ir=9∶1) | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 5 | 0.42 | 90.6 A·g-1 | [ |
PtIrNi1/SiO2-CNT (Pt∶Ir=9∶1) | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 5 | 0.399 | 124 A·g-1 | [ |
PtZn | 0.1 mol·L-1 NH3 + 0.5 mol·L-1 KOH | 100 | 0.42 | 0.60 mA·cm-2 ECSA | [ |
PtIrZn (Pt∶Ir=8∶2) | 0.1 mol·L-1 NH3 + 0.5 mol·L-1 KOH | 100 | 0.30 | 0.56 mA·cm-2 ECSA | [ |
CuPtRu (Pt∶Ru=7∶1) | 1 mol·L-1 KOH saturated with NH3 | 20 | 0.49 | 180 A·g-1 | [ |
PtIrZn2/CeO2-ZIF-8 | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 5 | 0.35 | 31.8 A·g-1 | [ |
PtIrZn2/SiO2-CNT-COOH | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 5 | 0.35 | 61.4 A·g-1 | [ |
PtIr/SiO2-CNT-COOH | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 5 | 0.33 | 64.6 A·g-1 | [ |
PtIrCu HCOND | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 5 | 0.35 | 122.9 A·g-1 | [ |
PtNi | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 10 | 0.69 | 75 A·g-1 | [ |
PtAu/C (Pt∶Au=7∶3) | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 20 | 0.51 | 90 A·g-1 | [ |
PtNi | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 10 | 约0.5 | 75.32 A·g-1 | [ |
Pt/C | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 50 | 约0.52② | 39.9 A·g-1 | [ |
PtNi/C | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 50 | 约0.55② | 76.4 A·g-1 | [ |
PtNiO/C | 0.1 mol·L-1 NH3 + 1 mol·L-1 KOH | 50 | 约0.55② | 86.9 A·g-1 | [ |
Ni98Pd2 | 0.5 mol·L-1 NaNO3 + 0.2 mol·L-1 NH4NO3 | 50 | 1.3① | 150 A·g-1 | [ |
NiCu/C | 55 m mol·L-1 NH4Cl + 0.5 mol·L-1 NaOH | 25 | 0.47② | 52 mA·cm-2 | [ |
NiCu/C | 0.5 mol·L-1 NH3 + 1 mol·L-1 KOH | 50 | 0.4① | 110.4 mA·cm-2 | [ |
NiCu/C | 55 m mol·L-1 NH4Cl + 0.5 mol·L-1 NaOH | 25 | 0.43① | 105 mA·cm-2 | [ |
Ni(OH)2/C | 55 m mol·L-1 NH4Cl + 0.5 mol·L-1 NaOH | 25 | 0.43① | 15 mA·cm-2 | [ |
NiCr/C | 55 m mol·L-1 NH4Cl + 0.5 mol·L-1 NaOH | 25 | 0.40① | 10 mA·cm-2 | [ |
NiMn/C | 55 m mol·L-1 NH4Cl + 0.5 mol·L-1 NaOH | 25 | 0.40① | 20 mA·cm-2 | [ |
NiCo/C | 55 m mol·L-1 NH4Cl + 0.5 mol·L-1 NaOH | 25 | 0.35① | 10 mA·cm-2 | [ |
NiZn/C | 55 m mol·L-1 NH4Cl + 0.5 mol·L-1 NaOH | 25 | 0.45① | 2 mA·cm-2 | [ |
Ni(OH)2 on NiOOH | 0.1 mol·L-1 NaSO4 + 0.003 mol·L-1 NH3 | 10 | 0.6① | 2.7 mA·cm-2 | [ |
①vs Hg/HgO。 ②vs Ag/AgCl。 |
膜 | 燃料 | 阳极催化剂 | 阴极催化剂 | 温度/℃ | 峰值功率密度/ (mW·cm-2) | 文献 |
---|---|---|---|---|---|---|
AEM (PAP-TP) | 3 mol·L-1 NH3 3 mol·L-1 KOH | PtIr/C 2 mg PGM·cm-2 | Acta 4020 1 mg·cm-2 | 80 | 135 | [ |
AEM (PAP-TP) | 7 mol·L-1 NH3 1.25 mol·L-1 KOH | PtIr/C 2 mg PGM·cm-2 | Acta 4020 1 mg·cm-2 | 95 | 390 (0.2 MPa) | [ |
AEM (PAP-TP) | 7 mol·L-1 NH3 1.25 mol·L-1 KOH | PtIr/C 2 mg PGM·cm-2 | Pd/C 0.4 mg·cm-2 | 95 | 304 (0.2 MPa) | [ |
AEM | NH3 | Pt/C 2 mg Pt·cm-2 | PGM-free | 100 | 420 | [ |
HEM (AHA) | 0.2 mol·L-1 NH3 1 mol·L-1 KOH | Pt/C 0.6 mg Pt·cm-2 | Pt/C 0.6 mg Pt·cm-2 | 80 | 0.22 | [ |
HEM (CPPO-PVA) | NH3 | Cr-Ni/C 10 mg·cm-2 | MnO2/C 20 mg·cm-2 | 25 | 11 | [ |
HEM (Resin-PVA) | 35% NH3 | Cr-Ni/C 10 mg·cm-2 | MnO2/C 20 mg·cm-2 | 25 | 9 | [ |
HEM (AMI-7001) | NH3 | Pt/C 0.45 mg Pt·cm-2 | Pt/C 0.45 mg Pt·cm-2 | 65 | 0.26 | [ |
HEM (AMI-7001) | 1 mol·L-1 NH3 | Pt/C 0.45 mg Pt·cm-2 | Pt/C 0.45 mg Pt·cm-2 | 25 | 0.71 | [ |
Mg-Al-CO32- LDH | 5 mol·L-1 MH3 1 mol·L-1 KOH | PtRu 3.3 mg·cm-2 | Pt/C | 80 | 4.5 | [ |
FAA AEM | 35% NH3 1 mol·L-1 KOH | NiCu/C 2.5 mg·cm-2 | SrCo0.8Cu0.1 Nb0.1O3-δ 18.67 mg·cm-2 | 25 | 0.25 | [ |
PAP-TP | NH3 + N2 | PtIr 2 mg PGM·cm-2 | Fe-N-C 3 mg·cm-2 | 95 | 75 | [ |
Tokuyama membrance | 16 mol·L-1 NH3 | Pt1Ir10 2 mg PGM·cm-2 | Ag 2 mg·cm-2 | 120 | 180 | [ |
Tokuyama membrance | 12 mol·L-1 NH3 2.5 mol·L-1 KOH | Pt1Ir10 2 mg PGM·cm-2 | Ag 2 mg·cm-2 | 100 | 280 | [ |
AEM (A201) | NH3 | Pt/C 0.5 mg Pt·cm-2 | Pt/C 0.5 mg Pt·cm-2 | 50 | 4.76 | [ |
AEM (A201) | NH3 | PtRu/C 0.5 mg Pt·cm-2 | Pt/C 0.5 mg Pt·cm-2 | 50 | 3.07 | [ |
AEM (A201) | NH3 | SnO2-Pt/C 0.4 mg Pt·cm-2 | Pt/C 0.4 mg Pt·cm-2 | 50 | 4.15 | [ |
Table 3 AEM-DAFC performance with various catalysts
膜 | 燃料 | 阳极催化剂 | 阴极催化剂 | 温度/℃ | 峰值功率密度/ (mW·cm-2) | 文献 |
---|---|---|---|---|---|---|
AEM (PAP-TP) | 3 mol·L-1 NH3 3 mol·L-1 KOH | PtIr/C 2 mg PGM·cm-2 | Acta 4020 1 mg·cm-2 | 80 | 135 | [ |
AEM (PAP-TP) | 7 mol·L-1 NH3 1.25 mol·L-1 KOH | PtIr/C 2 mg PGM·cm-2 | Acta 4020 1 mg·cm-2 | 95 | 390 (0.2 MPa) | [ |
AEM (PAP-TP) | 7 mol·L-1 NH3 1.25 mol·L-1 KOH | PtIr/C 2 mg PGM·cm-2 | Pd/C 0.4 mg·cm-2 | 95 | 304 (0.2 MPa) | [ |
AEM | NH3 | Pt/C 2 mg Pt·cm-2 | PGM-free | 100 | 420 | [ |
HEM (AHA) | 0.2 mol·L-1 NH3 1 mol·L-1 KOH | Pt/C 0.6 mg Pt·cm-2 | Pt/C 0.6 mg Pt·cm-2 | 80 | 0.22 | [ |
HEM (CPPO-PVA) | NH3 | Cr-Ni/C 10 mg·cm-2 | MnO2/C 20 mg·cm-2 | 25 | 11 | [ |
HEM (Resin-PVA) | 35% NH3 | Cr-Ni/C 10 mg·cm-2 | MnO2/C 20 mg·cm-2 | 25 | 9 | [ |
HEM (AMI-7001) | NH3 | Pt/C 0.45 mg Pt·cm-2 | Pt/C 0.45 mg Pt·cm-2 | 65 | 0.26 | [ |
HEM (AMI-7001) | 1 mol·L-1 NH3 | Pt/C 0.45 mg Pt·cm-2 | Pt/C 0.45 mg Pt·cm-2 | 25 | 0.71 | [ |
Mg-Al-CO32- LDH | 5 mol·L-1 MH3 1 mol·L-1 KOH | PtRu 3.3 mg·cm-2 | Pt/C | 80 | 4.5 | [ |
FAA AEM | 35% NH3 1 mol·L-1 KOH | NiCu/C 2.5 mg·cm-2 | SrCo0.8Cu0.1 Nb0.1O3-δ 18.67 mg·cm-2 | 25 | 0.25 | [ |
PAP-TP | NH3 + N2 | PtIr 2 mg PGM·cm-2 | Fe-N-C 3 mg·cm-2 | 95 | 75 | [ |
Tokuyama membrance | 16 mol·L-1 NH3 | Pt1Ir10 2 mg PGM·cm-2 | Ag 2 mg·cm-2 | 120 | 180 | [ |
Tokuyama membrance | 12 mol·L-1 NH3 2.5 mol·L-1 KOH | Pt1Ir10 2 mg PGM·cm-2 | Ag 2 mg·cm-2 | 100 | 280 | [ |
AEM (A201) | NH3 | Pt/C 0.5 mg Pt·cm-2 | Pt/C 0.5 mg Pt·cm-2 | 50 | 4.76 | [ |
AEM (A201) | NH3 | PtRu/C 0.5 mg Pt·cm-2 | Pt/C 0.5 mg Pt·cm-2 | 50 | 3.07 | [ |
AEM (A201) | NH3 | SnO2-Pt/C 0.4 mg Pt·cm-2 | Pt/C 0.4 mg Pt·cm-2 | 50 | 4.15 | [ |
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