Chinese Journal of Catalysis ›› 2021, Vol. 42 ›› Issue (8): 1360-1369.DOI: 10.1016/S1872-2067(20)63682-8
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Mathias Smialkowskia, David Tetzlaffa,b, Lars Hensgenc, Daniel Siegmundb, Ulf-Peter Apfela,b,*()
Received:
2020-03-30
Accepted:
2020-03-30
Online:
2021-08-18
Published:
2020-11-23
Contact:
Ulf-Peter Apfel
About author:
*. E-Mail: ulf.apfel@rub.de, ulf.apfel@umsicht.fraunhofer.de† Contributed equally to this work.
Supported by:
Mathias Smialkowski, David Tetzlaff, Lars Hensgen, Daniel Siegmund, Ulf-Peter Apfel. Fe/Co and Ni/Co-pentlandite type electrocatalysts for the hydrogen evolution reaction[J]. Chinese Journal of Catalysis, 2021, 42(8): 1360-1369.
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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63682-8
Fig. 2. DSC curves for the synthesized Fe/Co (A) as well as Ni/Co materials (B). DSC results for Co9S8 are added for comparison. Heating was performed from RT to 1000 °C with a rate of 10 °C min-1.
Fig. 3. ECSA slopes before (grey) and after (green) chronoamperometry at -400 mV vs. RHE (A) and recorded overpotentials before (grey) and after (green) chronoamperometry (B). The green bars indicate the difference between the respective data points.
Estimated sum formula | Fe equiv. | Co equiv. | Ni equiv. | S equiv. | Composition obtained from EDX analysis |
---|---|---|---|---|---|
Ni4.5Co4.5S8 | — | 5.33 | 4.94 | 6.73 | Co5.33Ni4.94S6.73 |
Ni3Co6S8 | — | 6.51 | 3.44 | 7.05 | Co6.51Ni3.44S7.05 |
Ni2Co7S8 | — | 7.17 | 1.92 | 7.91 | Co7.17Ni1.92S7.91 |
NiCo8S8 | — | 8.01 | 0.92 | 8.06 | Co8.01Ni0.92S8.06 |
Co9S8 | — | 9.01 | — | 7.99 | Co9.01S7.99 |
FeCo8S8 | 0.70 | 7.91 | — | 8.40 | Fe0.70Co7.91S8.40 |
Fe2Co7S8 | 2.64 | 7.24 | — | 7.12 | Fe2.64Co7.24S7.12 |
Fe3Co6S8 | 2.77 | 6.32 | — | 7.91 | Fe2.77Co6.32S7.91 |
Fe4.5Co4.5S8 | 4.01 | 8.04 | — | 4.96 | Fe4.01Co8.04S4.96 |
Table 1 Comparison of expected stoichiometry and obtained elemental composition from EDX. Elemental compositions from EDX are derived from at least 4 independent measurements.
Estimated sum formula | Fe equiv. | Co equiv. | Ni equiv. | S equiv. | Composition obtained from EDX analysis |
---|---|---|---|---|---|
Ni4.5Co4.5S8 | — | 5.33 | 4.94 | 6.73 | Co5.33Ni4.94S6.73 |
Ni3Co6S8 | — | 6.51 | 3.44 | 7.05 | Co6.51Ni3.44S7.05 |
Ni2Co7S8 | — | 7.17 | 1.92 | 7.91 | Co7.17Ni1.92S7.91 |
NiCo8S8 | — | 8.01 | 0.92 | 8.06 | Co8.01Ni0.92S8.06 |
Co9S8 | — | 9.01 | — | 7.99 | Co9.01S7.99 |
FeCo8S8 | 0.70 | 7.91 | — | 8.40 | Fe0.70Co7.91S8.40 |
Fe2Co7S8 | 2.64 | 7.24 | — | 7.12 | Fe2.64Co7.24S7.12 |
Fe3Co6S8 | 2.77 | 6.32 | — | 7.91 | Fe2.77Co6.32S7.91 |
Fe4.5Co4.5S8 | 4.01 | 8.04 | — | 4.96 | Fe4.01Co8.04S4.96 |
Compound | η before Chronoamperometry (mV) | η after Chronoamperometry (mV) | |Δη| (mV) | ECSA before Chronoamperometry (mA s cm-2 mV-1) | ECSA after Chronoamperometry (mA s cm-2 mV-1) | ΔECSA (mA s cm-2 mV-1) |
---|---|---|---|---|---|---|
Ni4.5Co4.5S8 | 336 | 293 | 43 | 0.00823 | 0.01546 | 0.00723 |
Ni3Co6S8 | 256 | 283 | 27 | 0.01539 | 0.02313 | 0.00774 |
Ni2Co7S8 | 334 | 347 | 13 | 0.00442 | 0.00805 | 0.00363 |
NiCo8S8 | 345 | 328 | 17 | 0.01032 | 0.01714 | 0.00682 |
Co9S8 | 333 | 319 | 14 | 0.01128 | 0.01996 | 0.00869 |
FeCo8S8 | 334 | 348 | 14 | 0.00241 | 0.00841 | 0.00599 |
Fe2Co7S8 | 357 | 352 | 5 | 0.00886 | 0.01021 | 0.00135 |
Fe3Co6S8 | 354 | 296 | 58 | 0.00109 | 0.00642 | 0.00532 |
Fe4.5Co4.5S8 | 327 | 286 | 41 | 0.00620 | 0.02800 | 0.02180 |
Table 2 Overpotentials and ECSA before and after chronoamperometry at -400 mV vs. RHE and 25 °C.
Compound | η before Chronoamperometry (mV) | η after Chronoamperometry (mV) | |Δη| (mV) | ECSA before Chronoamperometry (mA s cm-2 mV-1) | ECSA after Chronoamperometry (mA s cm-2 mV-1) | ΔECSA (mA s cm-2 mV-1) |
---|---|---|---|---|---|---|
Ni4.5Co4.5S8 | 336 | 293 | 43 | 0.00823 | 0.01546 | 0.00723 |
Ni3Co6S8 | 256 | 283 | 27 | 0.01539 | 0.02313 | 0.00774 |
Ni2Co7S8 | 334 | 347 | 13 | 0.00442 | 0.00805 | 0.00363 |
NiCo8S8 | 345 | 328 | 17 | 0.01032 | 0.01714 | 0.00682 |
Co9S8 | 333 | 319 | 14 | 0.01128 | 0.01996 | 0.00869 |
FeCo8S8 | 334 | 348 | 14 | 0.00241 | 0.00841 | 0.00599 |
Fe2Co7S8 | 357 | 352 | 5 | 0.00886 | 0.01021 | 0.00135 |
Fe3Co6S8 | 354 | 296 | 58 | 0.00109 | 0.00642 | 0.00532 |
Fe4.5Co4.5S8 | 327 | 286 | 41 | 0.00620 | 0.02800 | 0.02180 |
Fig. 5. ECSA slopes before (grey) and after (green) chronoamperometry at -400 mV vs. RHE (A) and recorded overpotentials before (grey) and after (green) chronoamperometry (B) with green bar graphs indicating the difference between the respective data points. All values obtained at 75 °C cell temperature.
Compound | η before Chronoamperometry (mV) | η after Chronoamperometry (mV) | |Δη| (mV) | ECSA before Chronoamperometry (mA s cm-2 mV-1) | ECSA after Chronoamperometry (mA s cm-2 mV-1) | ΔECSA (mA s cm-2 mV-1) |
---|---|---|---|---|---|---|
Ni4.5Co4.5S8 | 213 | 207 | 6 | 0.00845 | 0.01162 | 0.00318 |
Ni3Co6S8 | 182 | 192 | 10 | 0.02248 | 0.02786 | 0.00538 |
Ni2Co7S8 | 239 | 200 | 39 | 0.01067 | 0.02626 | 0.01559 |
NiCo8S8 | 246 | 233 | 13 | 0.00984 | 0.01276 | 0.00291 |
Co9S8 | 247 | 252 | 5 | 0.01193 | 0.01538 | 0.00346 |
FeCo8S8 | 270 | 278 | 8 | 0.00546 | 0.00894 | 0.00348 |
Fe2Co7S8 | 241 | 235 | 6 | 0.01097 | 0.01937 | 0.00840 |
Fe3Co6S8 | 227 | 239 | 12 | 0.00721 | 0.01250 | 0.00529 |
Fe4.5Co4.5S8 | 192 | 176 | 16 | 0.01919 | 0.04440 | 0.02521 |
Table 3 Values for overpotential and ECSA before and after chronoamperometry at -400 mV vs. RHE and 75 °C.
Compound | η before Chronoamperometry (mV) | η after Chronoamperometry (mV) | |Δη| (mV) | ECSA before Chronoamperometry (mA s cm-2 mV-1) | ECSA after Chronoamperometry (mA s cm-2 mV-1) | ΔECSA (mA s cm-2 mV-1) |
---|---|---|---|---|---|---|
Ni4.5Co4.5S8 | 213 | 207 | 6 | 0.00845 | 0.01162 | 0.00318 |
Ni3Co6S8 | 182 | 192 | 10 | 0.02248 | 0.02786 | 0.00538 |
Ni2Co7S8 | 239 | 200 | 39 | 0.01067 | 0.02626 | 0.01559 |
NiCo8S8 | 246 | 233 | 13 | 0.00984 | 0.01276 | 0.00291 |
Co9S8 | 247 | 252 | 5 | 0.01193 | 0.01538 | 0.00346 |
FeCo8S8 | 270 | 278 | 8 | 0.00546 | 0.00894 | 0.00348 |
Fe2Co7S8 | 241 | 235 | 6 | 0.01097 | 0.01937 | 0.00840 |
Fe3Co6S8 | 227 | 239 | 12 | 0.00721 | 0.01250 | 0.00529 |
Fe4.5Co4.5S8 | 192 | 176 | 16 | 0.01919 | 0.04440 | 0.02521 |
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