Photocatalytic NH3 versus H2 evolution over g-C3N4/CsxWO3: O2 and methanol tipping the scale

Anye Shi; Huihui Li; Shu Yin; Zaili Hou; Jiayue Rong; Jiachi Zhang; Yuhua Wang

doi:10.1016/j.apcatb.2018.04.081

Photocatalytic NH₃ versus H₂ evolution over g-C₃N₄/Cs_xWO₃: O₂ and methanol tipping the scale

Anye Shi, Huihui Li, Shu Yin, Zaili Hou, Jiayue Rong, Jiachi Zhang, Yuhua Wang

Research output: Contribution to journal › Article › peer-review

41 Citations (Scopus)

Abstract

Cs_xWO₃ nanorods can be used to sensitize the single layer g-C₃N₄, where full spectrum light harvesting excited electrons to drive the photocatalytic reduction of N₂ into NH₃. Under UV light, both water splitting and solar ammonia synthesis reaction exhibit high activity. However, selectivity towards ammonia over hydrogen is realized under NIR irradiation. With the control of methanol, O₂ can directly decide the NH₃ or H₂ evolution on photocatalyst. The origin is the strong capture of O₂ with the electrons from the photocatalyst under light irradiation to yield the oxygen active species, which transfer electrons subsequently with help of methanol to generate NH₃. However, H₂ production will be suppressed by O₂. And with its sacrifice, methanol preserves the produced NH₃ from oxidation. The O₂-sacrificial agent mediated NH₃ evolution reaction found here provides insights in the promotion role of them in other catalysis.

Original language	English
Pages (from-to)	197-206
Number of pages	10
Journal	Applied Catalysis B: Environmental
Volume	235
DOIs	https://doi.org/10.1016/j.apcatb.2018.04.081
Publication status	Published - 2018 Nov 5

Keywords

H evolution
N fixation
O content
Photocatalysis
Sacrificial agent

ASJC Scopus subject areas

Catalysis
Environmental Science(all)
Process Chemistry and Technology

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1016/j.apcatb.2018.04.081

Cite this

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title = "Photocatalytic NH3 versus H2 evolution over g-C3N4/CsxWO3: O2 and methanol tipping the scale",

abstract = "CsxWO3 nanorods can be used to sensitize the single layer g-C3N4, where full spectrum light harvesting excited electrons to drive the photocatalytic reduction of N2 into NH3. Under UV light, both water splitting and solar ammonia synthesis reaction exhibit high activity. However, selectivity towards ammonia over hydrogen is realized under NIR irradiation. With the control of methanol, O2 can directly decide the NH3 or H2 evolution on photocatalyst. The origin is the strong capture of O2 with the electrons from the photocatalyst under light irradiation to yield the oxygen active species, which transfer electrons subsequently with help of methanol to generate NH3. However, H2 production will be suppressed by O2. And with its sacrifice, methanol preserves the produced NH3 from oxidation. The O2-sacrificial agent mediated NH3 evolution reaction found here provides insights in the promotion role of them in other catalysis.",

keywords = "H evolution, N fixation, O content, Photocatalysis, Sacrificial agent",

author = "Anye Shi and Huihui Li and Shu Yin and Zaili Hou and Jiayue Rong and Jiachi Zhang and Yuhua Wang",

note = "Funding Information: This research was supported by the National Natural Science Foundation of China ( 51402139 ). Thanks to the partial supporting from the JSPS KAKENHI Grant Number JP16H06439 (Grant-in-Aid for Scientiﬁc Research on Innovative Areas), the Dynamic Alliance for Open Innovation Bridging Human, Environment and Materials , the Cooperative Research Program of “Network Joint Research Center for Materials and Devices” . ",

year = "2018",

month = nov,

day = "5",

doi = "10.1016/j.apcatb.2018.04.081",

language = "English",

volume = "235",

pages = "197--206",

journal = "Applied Catalysis B: Environmental",

issn = "0926-3373",

publisher = "Elsevier",

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TY - JOUR

T1 - Photocatalytic NH3 versus H2 evolution over g-C3N4/CsxWO3

T2 - O2 and methanol tipping the scale

AU - Shi, Anye

AU - Li, Huihui

AU - Yin, Shu

AU - Hou, Zaili

AU - Rong, Jiayue

AU - Zhang, Jiachi

AU - Wang, Yuhua

N1 - Funding Information: This research was supported by the National Natural Science Foundation of China ( 51402139 ). Thanks to the partial supporting from the JSPS KAKENHI Grant Number JP16H06439 (Grant-in-Aid for Scientiﬁc Research on Innovative Areas), the Dynamic Alliance for Open Innovation Bridging Human, Environment and Materials , the Cooperative Research Program of “Network Joint Research Center for Materials and Devices” .

PY - 2018/11/5

Y1 - 2018/11/5

N2 - CsxWO3 nanorods can be used to sensitize the single layer g-C3N4, where full spectrum light harvesting excited electrons to drive the photocatalytic reduction of N2 into NH3. Under UV light, both water splitting and solar ammonia synthesis reaction exhibit high activity. However, selectivity towards ammonia over hydrogen is realized under NIR irradiation. With the control of methanol, O2 can directly decide the NH3 or H2 evolution on photocatalyst. The origin is the strong capture of O2 with the electrons from the photocatalyst under light irradiation to yield the oxygen active species, which transfer electrons subsequently with help of methanol to generate NH3. However, H2 production will be suppressed by O2. And with its sacrifice, methanol preserves the produced NH3 from oxidation. The O2-sacrificial agent mediated NH3 evolution reaction found here provides insights in the promotion role of them in other catalysis.

AB - CsxWO3 nanorods can be used to sensitize the single layer g-C3N4, where full spectrum light harvesting excited electrons to drive the photocatalytic reduction of N2 into NH3. Under UV light, both water splitting and solar ammonia synthesis reaction exhibit high activity. However, selectivity towards ammonia over hydrogen is realized under NIR irradiation. With the control of methanol, O2 can directly decide the NH3 or H2 evolution on photocatalyst. The origin is the strong capture of O2 with the electrons from the photocatalyst under light irradiation to yield the oxygen active species, which transfer electrons subsequently with help of methanol to generate NH3. However, H2 production will be suppressed by O2. And with its sacrifice, methanol preserves the produced NH3 from oxidation. The O2-sacrificial agent mediated NH3 evolution reaction found here provides insights in the promotion role of them in other catalysis.

KW - H evolution

KW - N fixation

KW - O content

KW - Photocatalysis

KW - Sacrificial agent

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