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| 1 | Suppressing the liquid product crossover in electrochemical CO_(2)reduction显示文摘Coupling electrochemical CO_(2)reduction(CO_(2)R)with a renewable energy source to create high‐value fuels and chemicals is a promising strategy in moving toward a sustainable global energy economy.CO_(2)R liquid products,such as formate,acetate,ethanol,and propanol,offer high volumetric energy density and are more easily stored and transported than their gaseous coun-terparts.However,a significant amount(~30%)of liquid products from electrochemical CO_(2)R in a flow cell reactor cross the ion exchange membrane,leading to the substantial loss of system‐level Faradaic efficiency.This severe crossover of the liquid product has—until now—received limited attention.Here,we review promising methods to suppress liquid product crossover,including the use of bipolar membranes,solid‐state electrolytes,and cation‐exchange membranes‐based acidic CO_(2)R systems.We then outline the re-maining challenges and future prospects for the production of concentrated liquid products from CO_(2). | Ning Wang Rui Kai Miao Geonhui Lee Alberto Vomiero David Sinton Alexander H.Ip Hongyan Liang Edward H.Sargent | 2021 | SmartMat2021，2，1： | 13 |
| 2 | All-Perovskite Tandem Solar Cells:A Roadmap to Uniting High Efficiency with High Stability显示文摘CONSPECTUS:Organic−inorganic halide perovskite photovoltaics(PVs)only a decade-old fieldhave reached impressive power conversion efficiencies(PCEs)and passed industrial stability requirements(IEC 61215:2016 Damp Heat and Humidity Freeze tests),solidifying their status among candidates for next generation PVs.Among the various perovskite PV technologies,all-perovskite tandem solar cells(PTSCs)are frontrunners for commercialization.PTSCs unite a narrow-bandgap(NBG;Eg≈1.2 eV)perovskite back cell with a wide-bandgap(WBG;Eg≈1.7−1.9 eV)perovskite front cell.Despite their nascency,PTSCs have achieved certified PCEs of 24.8%and 24.2%for small-area(0.049 cm^2)and large-area devices(1.041 cm2),respectively.With further advances in materials development,PTSCs are capable of moving beyond the PCE limits of single-junction cells due to reduced thermalization losses and improved utilization of the solar spectrum.By contrast,the PCE of single-junction perovskite devices is already approaching its saturation level,which is already very close to the device’s Shockley−Queisser limit for a bandgap of around 1.55 eV.The tandem architecture,thus,provides the most viable path forward to further exploiting the potential of perovskite solar cells.However,PTSC technology faces a set of challenges distinct from those in perovskite single-junction devices because(i)NBG perovskitestypically achieved by Pb−Sn alloyingare prone to oxidation(Sn^2+to Sn^4+),which results in a high density of Sn vacancies that degrade the optoelectronic performance of NBG perovskite films,(ii)practically complete photon absorption and charge extraction require thick,NBG perovskite films having long carrier diffusion lengths,and(iii)WBG perovskites with high Br/(I+Br)ratio experience large voltage losses and inferior light stability due to surface trap states and phase segregation.In this Account,we discuss how to manage these considerations and maximize the power output in PTSCs via light management.We then review strategies,including composition-and additive-engineering,defect passivation,and matching charge transport layers,for enhancing the carrier diffusion length of NBG perovskite cells and mitigating voltage losses in WBG perovskite cells.We also summarize the advances made in the fabrication of PTSCs on the device level,especially the evolution of tunnel recombination junctions and tandem device architectures.Finally,we highlight further research efforts needed to overcome roadblocks to commercialization(e.g.,improving the environmental,thermal,and operating stability of these devices)and offer our perspective on the future development of this rapidly advancing field. | Xiaopeng Zheng Abdullah Y.Alsalloum Yi Hou Edward H.Sargent Osman M.Bakr | 2020 | Accounts of Materials Research2020，1，1： | 2 |
| 3 | Single-step-fabricated disordered metasurfaces for enhanced light extraction from LEDs显示文摘While total internal reflection(TIR)lays the foundation for many important applications,foremost fibre optics that revolutionised information technologies,it is undesirable in some other applications such as light-emitting diodes(LEDs),which are a backbone for energy-efficient light sources.In the case of LEDs,TIR prevents photons from escaping the constituent high-index materials.Advances in material science have led to good efficiencies in generating photons from electron–hole pairs,making light extraction the bottleneck of the overall efficiency of LEDs.In recent years,the extraction efficiency has been improved,using nanostructures at the semiconductor/air interface that outcouple trapped photons to the outside continuum.However,the design of geometrical features for light extraction with sizes comparable to or smaller than the optical wavelength always requires sophisticated and timeconsuming fabrication,which causes a gap between lab demonstration and industrial-level applications.Inspired by lightning bugs,we propose and realise a disordered metasurface for light extraction throughout the visible spectrum,achieved with single-step fabrication.By applying such a cost-effective light extraction layer,we improve the external quantum efficiency by a factor of 1.65 for commercialised GaN LEDs,demonstrating a substantial potential for global energy-saving and sustainability. | Peng Mao Changxu Liu Xiyan Li Mengxia Liu Qiang Chen Min Han Stefan A.Maier Edward H.Sargent Shuang Zhang | 2021 | Light(Science & Applications)2021，10，10： | 1 |
| 4 | All-perovskite tandems go bifacial显示文摘All-perovskite tandem cells are attractive candidates for next-generation photovoltaic technology as they hold the potential to combine high-efficiency with low weight and reduced energy-payback times.Now,researchers show that such tandem cells can be engineering to be bifacial,allowing them to utilize stray light reflected off the surrounding environment,resulting in a 17%boost in the power output. | Suhas Mahesh Bin Chen Edward H.Sargent | 2023 | Light(Science & Applications)2023，12，1： | 0 |
| 5 | Interpretable discovery of semiconductors with machine learning显示文摘Machine learning models of material properties accelerate materials discovery,reproducing density functional theory calculated results at a fraction of the cost1–6.To bridge the gap between theory and experiments,machine learning predictions need to be distilled in the form of interpretable chemical rules that can be used by experimentalists.Here we develop a framework to address this gap by combining evolutionary algorithm-powered search with machine-learning surrogate models.We then couple the search results with supervised learning and statistical testing.This strategy enables the efficient search of a materials space while providing interpretable design rules.We demonstrate its effectiveness by developing rules for the design of direct bandgap materials,stable UV emitters,and IR perovskite emitters.Finally,we conclusively show how DARWIN-generated rules are statistically more robust and applicable to a wide range of applications including the design of UV halide perovskites. | Hitarth Choubisa Petar Todorović Joao M.Pina Darshan H.Parmar Ziliang Li Oleksandr Voznyy Isaac Tamblyn Edward H.Sargent | 2023 | npj Computational Materials2023，，1： | 0 |
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