The 2022 solar fuels roadmap DOI Creative Commons
Gideon Segev, Jakob Kibsgaard, Christopher Hahn

et al.

Journal of Physics D Applied Physics, Journal Year: 2022, Volume and Issue: 55(32), P. 323003 - 323003

Published: May 13, 2022

Abstract Renewable fuel generation is essential for a low carbon footprint economy. Thus, over the last five decades, significant effort has been dedicated towards increasing performance of solar fuels generating devices. Specifically, to hydrogen efficiency photoelectrochemical cells progressed steadily its fundamental limit, and faradaic valuable products in CO 2 reduction systems increased dramatically. However, there are still numerous scientific engineering challenges that must be overcame order turn into viable technology. At electrode device level, conversion efficiency, stability selectivity significantly. Meanwhile, these metrics maintained when scaling up devices while maintaining an acceptable cost footprint. This roadmap surveys different aspects this endeavor: system benchmarking, scaling, various approaches photoelectrodes design, materials discovery, catalysis. Each sections focuses on single topic, discussing state art, key advancements required meet them. The can used as guide researchers funding agencies highlighting most pressing needs field.

Language: Английский

CO2 electroreduction to multicarbon products in strongly acidic electrolyte via synergistically modulating the local microenvironment DOI Creative Commons

Zesong Ma,

Zhilong Yang, Wenchuan Lai

et al.

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: Dec. 9, 2022

Electrochemical CO2 reduction to multicarbon products faces challenges of unsatisfactory selectivity, productivity, and long-term stability. Herein, we demonstrate electroreduction in strongly acidic electrolyte (pH ≤ 1) on electrochemically reduced porous Cu nanosheets by combining the confinement effect cation synergistically modulate local microenvironment. A Faradaic efficiency 83.7 ± 1.4% partial current density 0.56 0.02 cm-2, single-pass carbon 54.4%, stable electrolysis 30 h a flow cell are demonstrated for aqueous consisting sulfuric acid KCl with pH 1. Mechanistically, accumulated species (e.g., K+ OH-) Helmholtz plane account selectivity activity toward kinetically reducing proton coverage thermodynamically favoring conversion. We find that cations facilitate C-C coupling through interaction between key intermediate *OCCO.

Language: Английский

Citations

181
Conversion of CO2 to multicarbon products in strong acid by controlling the catalyst microenvironment DOI
Yong Zhao, Long Hao, Adnan Ozden

et al.

Nature Synthesis, Journal Year: 2023, Volume and Issue: unknown

Published: Feb. 9, 2023

Language: Английский

Citations

170
Durable CO2 conversion in the proton-exchange membrane system DOI

Wensheng Fang,

Wei Guo, Ruihu Lu

et al.

Nature, Journal Year: 2024, Volume and Issue: 626(7997), P. 86 - 91

Published: Jan. 31, 2024

Language: Английский

Citations

161
Multiscale CO2 Electrocatalysis to C2+ Products: Reaction Mechanisms, Catalyst Design, and Device Fabrication DOI
Tianxiang Yan, Xiaoyi Chen,

Lata Kumari

et al.

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(17), P. 10530 - 10583

Published: Aug. 17, 2023

Electrosynthesis of value-added chemicals, directly from CO2, could foster achievement carbon neutral through an alternative electrical approach to the energy-intensive thermochemical industry for utilization. Progress in this area, based on electrogeneration multicarbon products CO2 electroreduction, however, lags far behind that C1 products. Reaction routes are complicated and kinetics slow with scale up high levels required commercialization, posing significant problems. In review, we identify summarize state-of-art progress synthesis a multiscale perspective discuss current hurdles be resolved generation reduction including atomistic mechanisms, nanoscale electrocatalysts, microscale electrodes, macroscale electrolyzers guidelines future research. The review ends cross-scale links discrepancies between different approaches extensions performance stability issues arise industrial environment.

Language: Английский

Citations

138
Cation-Driven Increases of CO2 Utilization in a Bipolar Membrane Electrode Assembly for CO2 Electrolysis DOI Creative Commons
Kailun Yang, Mengran Li, Siddhartha Subramanian

et al.

ACS Energy Letters, Journal Year: 2021, Volume and Issue: 6(12), P. 4291 - 4298

Published: Nov. 11, 2021

Advancing reaction rates for electrochemical CO2 reduction in membrane electrode assemblies (MEAs) have boosted the promise of technology while exposing new shortcomings. Among these is maximum utilization CO2, which capped at 50% (CO as targeted product) due to unwanted homogeneous reactions. Using bipolar membranes an MEA (BPMEA) has capability preventing parasitic losses, but their dampened by poor activity and selectivity. In this work, we enable a 3-fold increase selectivity BPMEA system promoting alkali cation (K+) concentrations on catalyst's surface, achieving CO Faradaic efficiency 68%. When compared anion exchange membrane, cation-infused (BPM) shows 5-fold loss similar current densities, breaking mark. The work provides combined BPM strategy overcoming issues electrolyzers.

Language: Английский

Citations

136
Close to 90% Single-Pass Conversion Efficiency for CO2 Electroreduction in an Acid-Fed Membrane Electrode Assembly DOI
Binbin Pan, Fan Jia, Jie Zhang

et al.

ACS Energy Letters, Journal Year: 2022, Volume and Issue: 7(12), P. 4224 - 4231

Published: Oct. 31, 2022

The formation of (bi)carbonates is a pressing issue for CO2 electroreduction in neutral or alkaline solutions. It adversely causes low single-pass conversion efficiency as result (bi)carbonate crossover, well limited device lifetimes precipitation at the cathode. One emerging solution to circumvent this challenge conducting reaction acids. To end, we here demonstrate an acid-fed membrane electrode assembly (MEA) CO. A diluted electrolyte with H+ Cs+ ratio 1:1 and relatively current density are optimal conditions achieve high CO Faradaic efficiencies. versus offers electrocatalytic activities. By systematically evaluating impact concentration on electrochemical performance, uncover essential role balance between rates diffusion determining selectivity activity. As result, report partial ∼105 mA cm–2 ∼4 V cell voltage, near-doubled activity toward compared MEA similar voltage. Under long-term operation, our capable delivering ∼80%, extraordinary ∼90% (about twice that MEA), 50 h stability notably superior those previous reports.

Language: Английский

Citations

135
Engineering the NiNC Catalyst Microenvironment Enabling CO2 Electroreduction with Nearly 100% CO Selectivity in Acid DOI

Xuedi Sheng,

Wangxing Ge,

Hongliang Jiang

et al.

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(38)

Published: July 28, 2022

CO2 electrolysis in acid has emerged as a promising route to achieve high utilization due the inhibition of undesired carbonate formation that generally occurs alkaline or neutral conditions. However, efficiency and stability this system need be further improved through tailoring electrocatalyst its working environment. Here, microenvironment structurally engineered NiNC catalyst for acidic is probed optimized by adding hydrophobic poly(tetrafluoroethylene) (PTFE) nanoparticles catalytic layer gas-diffusion electrodes. The PTFE-modified electrode delivers nearly 100% CO Faradaic at an industry-relevant current density 250 mA cm-2 , single-pass 75.7% 200 under 20 sccm gas flow rate. Moreover, compared conventional without added PTFE, exhibits substantially enhanced water-flooding-resistant ability. Mechanistic investigations reveal moderate PTFE modification can optimize local /H2 O ratio layer, favoring reduction diffusion thickness highly active stable solid-liquid-gas interfacial microenvironment.

Language: Английский

Citations

128
Acidic CO2-to-HCOOH electrolysis with industrial-level current on phase engineered tin sulfide DOI Creative Commons
Haifeng Shen, Huanyu Jin, Haobo Li

et al.

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: May 18, 2023

Acidic CO2-to-HCOOH electrolysis represents a sustainable route for value-added CO2 transformations. However, competing hydrogen evolution reaction (HER) in acid remains great challenge selective production, especially industrial-level current densities. Main group metal sulfides derived S-doped metals have demonstrated enhanced selectivity alkaline and neutral media by suppressing HER tuning reduction intermediates. Yet stabilizing these sulfur dopants on surfaces at large reductive potentials HCOOH production is still challenging acidic medium. Herein, we report phase-engineered tin sulfide pre-catalyst (π-SnS) with uniform rhombic dodecahedron structure that can derive metallic Sn catalyst stabilized In situ characterizations theoretical calculations reveal the π-SnS has stronger intrinsic Sn-S binding strength than conventional phase, facilitating stabilization of residual species subsurface. These effectively modulate CO2RR intermediates coverage medium enhancing *OCHO intermediate adsorption weakening *H binding. As result, (Sn(S)-H) demonstrates significantly high Faradaic efficiency (92.15 %) carbon (36.43 to industrial densities (up -1 A cm-2)

Language: Английский

Citations

128
Efficient multicarbon formation in acidic CO2 reduction via tandem electrocatalysis DOI
Yuanjun Chen, Xiaoyan Li, Zhu Chen

et al.

Nature Nanotechnology, Journal Year: 2023, Volume and Issue: 19(3), P. 311 - 318

Published: Nov. 23, 2023

Language: Английский

Citations

120
Tailoring acidic microenvironments for carbon-efficient CO2electrolysis over a Ni–N–C catalyst in a membrane electrode assembly electrolyzer DOI
Hefei Li, Haobo Li, Pengfei Wei

et al.

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(4), P. 1502 - 1510

Published: Jan. 1, 2023

By tailoring the microenvironments of a Ni–N–C catalyst in an acidic MEA electrolyzer, we achieve CO faradaic efficiency 95% at 500 mA cm −2 , and 2 loss is reduced by 86% 300 pH 0.5, compared to alkaline electrolysis.

Language: Английский

Citations

111