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Zhao, Y., Ding, Y., Li, W., Liu, C., Li, Y., Zhao, Z., . . . Li, F. (2023). Efficient urea electrosynthesis from carbon dioxide and nitrate via alternating Cu–W bimetallic C–N coupling sites. Nature Communications, 14(1), Article ID 4491.
Open this publication in new window or tab >>Efficient urea electrosynthesis from carbon dioxide and nitrate via alternating Cu–W bimetallic C–N coupling sites
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2023 (English)In: Nature Communications, E-ISSN 2041-1723, Vol. 14, no 1, article id 4491Article in journal (Refereed) Published
Abstract [en]

Electrocatalytic urea synthesis is an emerging alternative technology to the traditional energy-intensive industrial urea synthesis protocol. Novel strategies are urgently needed to promote the electrocatalytic C–N coupling process and inhibit the side reactions. Here, we report a CuWO4 catalyst with native bimetallic sites that achieves a high urea production rate (98.5 ± 3.2 μg h−1 mg−1cat) for the co-reduction of CO2 and NO3− with a high Faradaic efficiency (70.1 ± 2.4%) at −0.2 V versus the reversible hydrogen electrode. Mechanistic studies demonstrated that the combination of stable intermediates of *NO2 and *CO increases the probability of C–N coupling and reduces the potential barrier, resulting in high Faradaic efficiency and low overpotential. This study provides a new perspective on achieving efficient urea electrosynthesis by stabilizing the key reaction intermediates, which may guide the design of other electrochemical systems for high-value C–N bond-containing chemicals.

Place, publisher, year, edition, pages
Springer Nature, 2023
National Category
Physical Chemistry
Identifiers
urn:nbn:se:kth:diva-335714 (URN)10.1038/s41467-023-40273-2 (DOI)001038216100018 ()37495582 (PubMedID)2-s2.0-85165918229 (Scopus ID)
Note

QC 20230912

Available from: 2023-09-12 Created: 2023-09-12 Last updated: 2024-03-15Bibliographically approved
Yang, H., Liu, Y., Ding, Y., Li, F., Wang, L., Cai, B., . . . Sun, L. (2023). Monolithic FAPbBr3 photoanode for photoelectrochemical water oxidation with low onset-potential and enhanced stability. Nature Communications, 14(1), Article ID 5486.
Open this publication in new window or tab >>Monolithic FAPbBr3 photoanode for photoelectrochemical water oxidation with low onset-potential and enhanced stability
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2023 (English)In: Nature Communications, E-ISSN 2041-1723, Vol. 14, no 1, article id 5486Article in journal (Refereed) Published
Abstract [en]

Despite considerable research efforts on photoelectrochemical water splitting over the past decades, practical application faces challenges by the absence of efficient, stable, and scalable photoelectrodes. Herein, we report a metal-halide perovskite-based photoanode for photoelectrochemical water oxidation. With a planar structure using mesoporous carbon as a hole-conducting layer, the precious metal-free FAPbBr3 photovoltaic device achieves 9.2% solar-to-electrical power conversion efficiency and 1.4 V open-circuit voltage. The photovoltaic architecture successfully applies to build a monolithic photoanode with the FAPbBr3 absorber, carbon/graphite conductive protection layers, and NiFe catalyst layers for water oxidation. The photoanode delivers ultralow onset potential below 0 V versus the reversible hydrogen electrode and high applied bias photon-to-current efficiency of 8.5%. Stable operation exceeding 100 h under solar illumination by applying ultraviolet-filter protection. The photothermal investigation verifies the performance boost in perovskite photoanode by photothermal effect. This study is significant in guiding the development of photovoltaic material-based photoelectrodes for solar fuel applications.

Place, publisher, year, edition, pages
Springer Nature, 2023
National Category
Materials Chemistry Physical Chemistry Other Physics Topics
Identifiers
urn:nbn:se:kth:diva-337792 (URN)10.1038/s41467-023-41187-9 (DOI)001065300300024 ()37679329 (PubMedID)2-s2.0-85170192499 (Scopus ID)
Note

QC 20231009

Available from: 2023-10-09 Created: 2023-10-09 Last updated: 2024-03-15Bibliographically approved
Yang, H., Li, F., Zhan, S., Liu, Y., Li, W., Meng, Q., . . . Sun, L. (2022). Intramolecular hydroxyl nucleophilic attack pathway by a polymeric water oxidation catalyst with single cobalt sites. Nature Catalysis, 5(5), 414-429
Open this publication in new window or tab >>Intramolecular hydroxyl nucleophilic attack pathway by a polymeric water oxidation catalyst with single cobalt sites
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2022 (English)In: Nature Catalysis, ISSN 2520-1158, Vol. 5, no 5, p. 414-429Article in journal (Refereed) Published
Abstract [en]

Exploration of efficient water oxidation catalysts (WOCs) is the primary challenge in conversion of renewable energy into fuels. Here we report a molecularly well-defined heterogeneous WOC with Aza-fused, pi-conjugated, microporous polymer (Aza-CMP) coordinated single cobalt sites (Aza-CMP-Co). The single cobalt sites in Aza-CMP-Co exhibited superior activity under alkaline and near-neutral conditions. Moreover, the molecular nature of the isolated catalytic sites makes Aza-CMP-Co a reliable model for studying the heterogeneous water oxidation mechanism. By a combination of experimental and theoretical results, a pH-dependent nucleophilic attack pathway for O-O bond formation was proposed. Under alkaline conditions, the intramolecular hydroxyl nucleophilic attack (IHNA) process with which the adjacent -OH group nucleophilically attacks Co4+=O was identified as the rate-determining step. This process leads to lower activation energy and accelerated kinetics than those of the intermolecular water nucleophilic attack (WNA) pathway. This study provides significant insights into the crucial function of electrolyte pH in water oxidation catalysis and enhancement of water oxidation activity by regulation of the IHNA pathway.

Place, publisher, year, edition, pages
Springer Nature, 2022
National Category
Physical Chemistry
Identifiers
urn:nbn:se:kth:diva-313755 (URN)10.1038/s41929-022-00783-6 (DOI)000801852700013 ()2-s2.0-85130755520 (Scopus ID)
Note

QC 20220613

Available from: 2022-06-13 Created: 2022-06-13 Last updated: 2024-03-15Bibliographically approved
Zhao, Z., Zhan, S., Feng, L., Liu, C., Ahlquist, M. S. G., Wu, X., . . . Sun, L. (2021). Molecular Engineering of Photocathodes based on Polythiophene Organic Semiconductors for Photoelectrochemical Hydrogen Generation. ACS Applied Materials and Interfaces, 13(34), 40602-40611
Open this publication in new window or tab >>Molecular Engineering of Photocathodes based on Polythiophene Organic Semiconductors for Photoelectrochemical Hydrogen Generation
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2021 (English)In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 13, no 34, p. 40602-40611Article in journal (Refereed) Published
Abstract [en]

Organic semiconductors provide significant potentials for the construction of photoelectrochemical (PEC) cells for solar hydrogen production because of their highly tunable properties. Herein, on carbon fiber paper (CFP) surface, pyridyl (Py), and 4,4'-bipyridin-1-ium (Py-2(+)) groups were introduced into polythiophene (pTH) semiconductor by electrochemical copolymerization, respectively. After assembly with the Co(dmgBF(2))(2) type catalyst (CoB, dmgBF(2) = difluoroboryldimethylglyoximate), the CoB@Py-2(+)-pTH/CFP photocathode displayed nearly twice the photocurrent enhancement (550 mu A cm(-2) at 0.15 V vs reversible hydrogen electrode, RHE) comparing to that generated by the CoB@Py-pTH/CFP photocathode (290 mu A cm(-2) at 0.15 V vs RHE) for light-driven H-2 generation under AM 1.5 solar illumination. Investigation of the mechanism revealed that the introduction of the positively charged pyridinium groups could improve the intrinsic Co(dmgBF(2))(2) catalyst activity for the H-2 generation reaction. Meanwhile, the positively charged pyridinium groups serve as p-type dopants to increase the semiconductor bulk charge transfer rate and act as electron transfer mediators to promote the interfacial charge transfer kinetics between the catalyst and the pTH-based organic semiconductor.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2021
Keywords
photocathode, polythiophene, photoelectrochemical (PEC) cell, light-driven hydrogen production, solar energy conversion
National Category
Other Chemistry Topics
Identifiers
urn:nbn:se:kth:diva-302609 (URN)10.1021/acsami.1c10561 (DOI)000693050200038 ()34403243 (PubMedID)2-s2.0-85114084978 (Scopus ID)
Note

QC 20211010

Available from: 2021-10-10 Created: 2021-10-10 Last updated: 2024-03-15Bibliographically approved
Meng, Q., Zhang, B., Yang, H., Liu, C., Li, Y., Kravchenko, O., . . . Sun, L. (2021). Remarkable synergy of borate and interfacial hole transporter on BiVO4 photoanodes for photoelectrochemical water oxidation. Materials Advances, 2(13), 4323-4332
Open this publication in new window or tab >>Remarkable synergy of borate and interfacial hole transporter on BiVO4 photoanodes for photoelectrochemical water oxidation
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2021 (English)In: Materials Advances, E-ISSN 2633-5409, Vol. 2, no 13, p. 4323-4332Article in journal (Refereed) Published
Abstract [en]

Bismuth vanadate (BiVO4) is one of the most fascinating building blocks for the design and assembly of highly efficient artificial photosynthesis devices for solar water splitting. Our recent report has shown that borate treated BiVO4 (B-BiVO4) results in an improved water oxidation performance. In this study, further improvement of both the photoelectrochemical (PEC) activity and stability of B-BiVO4 was successfully achieved by introducing NiFeV LDHs as an oxygen evolution catalyst and interfacial hole transporter. Benefiting from the synergistic effect of co-catalyst and borate pretreatment, the as-prepared NiFeV/B-BiVO4 exhibited a high photocurrent density of 4.6 mA cm−2 at 1.23 VRHE and an outstanding onset potential of ∼0.2 VRHE with good long-term stability. More importantly, NiFeV was found to play a pivotal role in the critically efficient suppression of charge combination on the BiVO4 surface and acceleration of charge transfer rather than a mere electrocatalyst for water oxidation.

National Category
Materials Chemistry
Research subject
Chemistry
Identifiers
urn:nbn:se:kth:diva-304228 (URN)10.1039/d1ma00344e (DOI)000657685300001 ()2-s2.0-85109312450 (Scopus ID)
Funder
Swedish Research CouncilKnut and Alice Wallenberg Foundation, KAW 2016.0072
Note

QC 20211117

Available from: 2021-10-28 Created: 2021-10-28 Last updated: 2024-03-15Bibliographically approved
Fang, Z., Zhang, P., Wang, M., Li, F., Wu, X., Fan, K. & Sun, L. (2021). Selective Electro-oxidation of Alcohols to the Corresponding Aldehydes in Aqueous Solution via Cu(III) Intermediates from CuO Nanorods. ACS Sustainable Chemistry and Engineering, 9(35), 11855-11861
Open this publication in new window or tab >>Selective Electro-oxidation of Alcohols to the Corresponding Aldehydes in Aqueous Solution via Cu(III) Intermediates from CuO Nanorods
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2021 (English)In: ACS Sustainable Chemistry and Engineering, E-ISSN 2168-0485, Vol. 9, no 35, p. 11855-11861Article in journal (Refereed) Published
Abstract [en]

Electrochemical oxidation using renewable energy is an attractive strategy that provides a sustainable and mild approach for biomass transformation. Herein, the electrocatalytic oxidation of furfuryl alcohol in an aqueous solution was investigated using CuO nanorods. Two kinds of Cu-III intermediates, namely, (CuO2)(-) and (Cu2O6)(6-), were detected on the surface of the working electrode. (Cu2O6)(6-), generated in the potential range of 1.35-1.39 V versus the reversible hydrogen electrode (RHE), induced the oxidation of furfuryl alcohol to furaldehyde with a yield of >= 98%. (CuO2)(-), generated at a potential greater than 1.39 V versus RHE, which led to the oxidation of furfuryl alcohol to 2-furoic acid with a yield of >= 99%. Furthermore, the Cu-III-catalyzed system exhibited a measure of universal applicability, wherein (Cu2O6)(6-) and (CuO2)(-) induced the highly selective electro-oxidation of benzyl alcohol, vanillyl alcohol, and 4-pyridinemethanol to yield the corresponding aldehydes and acids, respectively.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2021
Keywords
electrosynthesis, catalysts, oxidation, reaction mechanisms, biomass conversion
National Category
Materials Chemistry Organic Chemistry Other Chemistry Topics
Identifiers
urn:nbn:se:kth:diva-303064 (URN)10.1021/acssuschemeng.1c03691 (DOI)000695384700023 ()2-s2.0-85114693909 (Scopus ID)
Note

QC 20211005

Available from: 2021-10-05 Created: 2021-10-05 Last updated: 2024-03-15Bibliographically approved
Liu, C., Liu, T., Li, Y., Zhao, Z., Zhou, D., Li, W., . . . Li, Z. (2020). A dendritic Sb2Se3/In2S3 heterojunction nanorod array photocathode decorated with a MoSx catalyst for efficient solar hydrogen evolution. Journal of Materials Chemistry A, 8(44), 23385-23394
Open this publication in new window or tab >>A dendritic Sb2Se3/In2S3 heterojunction nanorod array photocathode decorated with a MoSx catalyst for efficient solar hydrogen evolution
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2020 (English)In: Journal of Materials Chemistry A, ISSN 2050-7488, E-ISSN 2050-7496, Vol. 8, no 44, p. 23385-23394Article in journal (Refereed) Published
Abstract [en]

Developing cost-effective photocathodes that show desirable performance for use in commercial photoelectrochemical water splitting devices remains a fundamental and practical challenge. Sb2Se3 semiconductors satisfy most of the demands expected for an ideal highly efficient photocathode, including favorable cost and optoelectronic properties. Herein, we have demonstrated outstanding photoelectrodes using a noble-metal-free catalyst, namely, a MoSx-decorated low-cost Sb2Se3/In2S3 heterojunction, as the photocathode. This enabled a maximum photocurrent density of up to -27 mA cm(-2) (0 V vs. RHE, 100 mW cm(-2), AM 1.5G filter) with a remarkable half solar-to-hydrogen conversion efficiency (STH) of 2.6%, obtained via decreasing charge recombination and accelerating charge transfer through morphological optimization of the In2S3 layer.

Place, publisher, year, edition, pages
Royal Society of Chemistry (RSC), 2020
National Category
Materials Chemistry
Identifiers
urn:nbn:se:kth:diva-287528 (URN)10.1039/d0ta08874a (DOI)000590158400021 ()2-s2.0-85096413830 (Scopus ID)
Note

QC 20210303

Available from: 2021-03-03 Created: 2021-03-03 Last updated: 2024-03-15Bibliographically approved
Li, F., Li, Y., Zhuo, Q., Zhou, D., Zhao, Y., Zhao, Z., . . . Sun, L. (2020). Electroless Plating of NiFeP Alloy on the Surface of Silicon Photoanode for Efficient Photoelectrochemical Water Oxidation. ACS Applied Materials and Interfaces, 12(10), 11479-11488
Open this publication in new window or tab >>Electroless Plating of NiFeP Alloy on the Surface of Silicon Photoanode for Efficient Photoelectrochemical Water Oxidation
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2020 (English)In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 12, no 10, p. 11479-11488Article in journal (Refereed) Published
Abstract [en]

N- type silicon is a kind of semiconductor with a narrow band gap that has been reported as an outstanding light-harvesting material for photoelectrochemical (PEC) reactions. Decorating a thin catalyst layer on the n-type silicon surface can provide a direct and effective route toward PEC water oxidation. However, most of catalyst immobilization methods for reported n-type silicon photoanodes have been based on energetically demanding, time-consuming, and high-cost processes. Herein, a high-performance NiFeP alloy (NiFeP)-decorated n-type micro-pyramid silicon array (n-Si) photoanode (NiFeP/n-Si) was prepared by a fast and low-cost electroless deposition method for light-driven water oxidation reaction. The saturated photocurrent density of NiFeP/n-Si can reach up to similar to 40 mA cm(-2) and a photocurrent density of 15.5 mA cm(-2) can be achieved at 1.23 V-RHE under light illumination (100 mW cm(-2), AM1.5 filter), which is one of the most promising silicon-based photoanodes to date. The kinetic studies showed that the NiFeP on the silicon photoanodes could significantly decrease the interfacial charge recombination between the n-type silicon surface and electrolyte.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2020
Keywords
silicon photoanode, electroless plating, photoelectrochemical cell, oxygen evolution reaction (OER), solar energy conversion
National Category
Organic Chemistry
Identifiers
urn:nbn:se:kth:diva-273105 (URN)10.1021/acsami.9b19418 (DOI)000526609100017 ()32056436 (PubMedID)2-s2.0-85080116249 (Scopus ID)
Note

QC 20200518

Available from: 2020-05-18 Created: 2020-05-18 Last updated: 2022-06-26Bibliographically approved
Li, W., Li, F., Yang, H., Wu, X., Zhang, P., Shan, Y. & Sun, L. (2019). A bio-inspired coordination polymer as outstanding water oxidation catalyst via second coordination sphere engineering. Nature Communications, 10, Article ID 5074.
Open this publication in new window or tab >>A bio-inspired coordination polymer as outstanding water oxidation catalyst via second coordination sphere engineering
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2019 (English)In: Nature Communications, E-ISSN 2041-1723, Vol. 10, article id 5074Article in journal (Refereed) Published
Abstract [en]

First-row transition metal-based catalysts have been developed for the oxygen evolution reaction (OER) during the past years, however, such catalysts typically operate at overpotentials (eta) significantly above thermodynamic requirements. Here, we report an iron/ nickel terephthalate coordination polymer on nickel form (NiFeCP/NF) as catalyst for OER, in which both coordinated and uncoordinated carboxylates were maintained after electrolysis. NiFeCP/NF exhibits outstanding electro-catalytic OER activity with a low overpotential of 188 mV at 10 mA cm(-2) in 1.0 KOH, with a small Tafel slope and excellent stability. The pH-independent OER activity of NiFeCP/NF on the reversible hydrogen electrode scale suggests that a concerted proton-coupled electron transfer (c-PET) process is the rate-determining step (RDS) during water oxidation. Deuterium kinetic isotope effects, proton inventory studies and atom-proton-transfer measurements indicate that the uncoordinated carboxylates are serving as the proton transfer relays, with a similar function as amino acid residues in photosystem II (PSII), accelerating the proton-transfer rate.

Place, publisher, year, edition, pages
NATURE PUBLISHING GROUP, 2019
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-264324 (URN)10.1038/s41467-019-13052-1 (DOI)000494938800001 ()31699987 (PubMedID)2-s2.0-85074684201 (Scopus ID)
Note

QC 20191202

Available from: 2019-12-02 Created: 2019-12-02 Last updated: 2024-03-15Bibliographically approved
Li, F., Xu, R., Nie, C., Wu, X., Zhang, P., Duan, L. & Sun, L. (2019). Dye-sensitized LaFeO3 photocathode for solar-driven H-2 generation. Chemical Communications, 55(86), 12940-12943
Open this publication in new window or tab >>Dye-sensitized LaFeO3 photocathode for solar-driven H-2 generation
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2019 (English)In: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, Vol. 55, no 86, p. 12940-12943Article in journal (Refereed) Published
Abstract [en]

Mesoporous LaFeO3 was used as a p-type visible-light-absorbing semiconductor (VLAS) substrate for light-driven H-2 generation. The successful modification of LaFeO3 with a molecular dye (P1*) and a molecular hydrogen production catalyst (NiP) paved a novel way to construct DS-PEC photocathodes for solar-driven H-2 generation by using VLASs.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2019
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-263680 (URN)10.1039/c9cc06781g (DOI)000492378600008 ()31599888 (PubMedID)2-s2.0-85074118816 (Scopus ID)
Note

QC 20191108

Available from: 2019-11-08 Created: 2019-11-08 Last updated: 2024-03-15Bibliographically approved
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Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0003-3455-0855

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