02515nas a2200301 4500008004100000022001400041245012200055210006900177260000800246300001200254490000700266520151500273653002101788653002401809653001901833653002301852100001801875700001901893700002201912700001601934700001501950700002701965700003301992700001802025700002302043700002502066856012202091 2022 eng d a0935-964800aMorphology-tuned Pt3Ge accelerates water dissociation to industrial-standard hydrogen production over a wide pH range0 aMorphologytuned Pt3Ge accelerates water dissociation to industri cJUL a22022940 v343 a

The discovery of novel materials for industrial-standard hydrogen production is the present need considering the global energy infrastructure. A novel electrocatalyst, Pt3Ge, which is engineered with a desired crystallographic facet (202), accelerates hydrogen production by water electrolysis, and records industrially desired operational stability compared to the commercial catalyst platinum is introduced. Pt3Ge-(202) exhibits low overpotential of 21.7 mV (24.6 mV for Pt/C) and 92 mV for 10 and 200 mA cm(-2) current density, respectively in 0.5 m H2SO4. It also exhibits remarkable stability of 15 000 accelerated degradation tests cycles (5000 for Pt/C) and exceptional durability of 500 h (@10 mA cm(-2)) in acidic media. Pt3Ge-(202) also displays low overpotential of 96 mV for 10 mA cm(-2) current density in the alkaline medium, rationalizing its hydrogen production ability over a wide pH range required commercial operations. Long-term durability (>75 h in alkaline media) with the industrial level current density (>500 mA cm(-2)) has been demonstrated by utilizing the electrochemical flow reactor. The driving force behind this stupendous performance of Pt3Ge-(202) has been envisaged by mapping the reaction mechanism, active sites, and charge-transfer kinetics via controlled electrochemical experiments, ex situ X-ray photoelectron spectroscopy, in situ infrared spectroscopy, and in situ X-ray absorption spectroscopy further corroborated by first principles calculations.

10aElectrochemistry10ahydrogen production10aintermetallics10awater electrolysis1 aMondal, Soumi1 aSarkar, Shreya1 aBagchi, Debabrata1 aDas, Tisita1 aDas, Risov1 aSingh, Ashutosh, Kumar1 aPrasanna, Ponnappa, Kechanda1 aVinod, C., P.1 aChakraborty, Sudip1 aPeter, Sebastian, C. uhttps://library.ncl.res.in/content/morphology-tuned-pt3ge-accelerates-water-dissociation-industrial-standard-hydrogen03019nas a2200301 4500008004100000022001400041245014600055210006900201260000900270300001600279490000700295520196300302653000902265653003202274653001802306653002302324653003802347653003002385653002502415100001802440700001602458700002202474700002002496700002702516700002802543700002502571856012102596 2023 eng d a1936-085100aDistortion-induced interfacial charge transfer at single cobalt atom secured on ordered intermetallic surface enhances pure oxygen production0 aDistortioninduced interfacial charge transfer at single cobalt a cNOV  a23169-231800 v173 a

In this work, atomic cobalt (Co) incorporation into the Pd2Ge intermetallic lattice facilitates operando generation of a thin layer of CoO over Co-substituted Pd2Ge, with Co in the CoO surface layer functioning as single metal sites. Hence the catalyst has been titled Co-1-CoO-Pd2Ge. High-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, and X-ray absorption spectroscopy confirm the existence of CoO, with some of the Co bonded to Ge by substitution of Pd sites in the Pd2Ge lattice. The role of the CoO layer in the oxygen evolution reaction (OER) has been verified by its selective removal using argon sputtering and conducting the OER on the etched catalyst. In situ X-ray absorption near-edge structure and extended X-ray absorption fine structure spectroscopy demonstrate that CoO gets transformed to CoOOH (Co3+) in operando condition with faster charge transfer through Pd atoms in the core Pd2Ge lattice. In situ Raman spectroscopy depicts the emergence of a CoOOH phase on applying potential and shows that the phase is stable with increasing potential and time without getting converted to CoO2. Density functional theory calculations indicate that the Pd2Ge lattice induces distortion in the CoO phase and generates unpaired spins in a nonmagnetic CoOOH system resulting in an increase in the OER activity and durability. The existence of spin density even after electrocatalysis is verified from electron paramagnetic resonance spectroscopy. We have thus successfully synthesized intermetallic supported CoO during synthesis and rigorously verified the role played by an intermetallic Pd2Ge core in enhancing charge transfer, generating spin density, improving electrochemical durability, and imparting mechanical stability to a thin CoOOH overlayer. Differential electrochemical mass spectrometry has been explored to visualize the instantaneous generation of oxygen gas during the onset of the reaction.

10aDEMS10ainterfacial charge transfer10aIntermetallic10along-termstability10aoperando spectroscopic techniques10aOxygen Evolution Reaction10astructuraldistortion1 aMondal, Soumi1 aRiyaz, Mohd1 aBagchi, Debabrata1 aDutta, Nilutpal1 aSingh, Ashutosh, Kumar1 aVinod, Chathakudath, P.1 aPeter, Sebastian, C. uhttps://library.ncl.res.in/content/distortion-induced-interfacial-charge-transfer-single-cobalt-atom-secured-ordered02464nas a2200325 4500008004100000245014900041210006900190260000800259300001500267490000700282520139000289653001501679653001501694653001801709653001101727653001601738653001901754100001601773700002601789700001901815700002701834700001501861700001801876700001601894700001901910700002001929700002801949700002501977856013602002 2025 eng d00aDopant and exfoliation induced simultaneous modification of charge density and C―C coupling sites for efficient CO2 photoreduction to ethylene0 aDopant and exfoliation induced simultaneous modification of char cJUL ae2024234710 v643 a

The photochemical conversion of CO2 into C2+ products has emerged as an attractive method for synthesizing valuable chemicals and fuels using abundant solar energy. However, the challenge lies in enhancing the efficiency and selectivity of C2+ product formation. In this study, we employed a heteroatom doping strategy to optimize the photocatalytic parameters and achieve excellent efficiency and selectivity in the photocatalytic CO2 reduction to C2+ product formation. Our experimental analysis revealed that the local electronic structure of the catalyst, modified by In-doping, enables enhanced efficiency. Additionally, the incorporation of Cu facilitates the coupling of C1 intermediates, resulting in excellent selectivity towards C2+ products. The CO2 reduction performance is further enhanced through exfoliation, which increases the exposure of active sites and extends the charge carrier lifetime by reducing the charge diffusion length. We report that the rate of formation of C2H4 reached 54.3 mu molh(-1)g(-1) with an outstanding selectivity of 91% over the exfoliated CuIn-doped AgBiP2S6 catalyst. By elucidating the role of heteroatom doping and exfoliation in enhancing both the efficiency and selectivity of C2+ product formation, our study contributes to advancing the development of sustainable and efficient photocatalytic CO2 conversion technologies.

10aC & horbar10aC coupling10aCO2 reduction10aDoping10aExfoliation10aPhotocatalysis1 aDas, Kousik1 aChakraborty, Subhajit1 aKediya, Siddhi1 aSingh, Ashutosh, Kumar1 aDas, Risov1 aMondal, Soumi1 aRiyaz, Mohd1 aGoud, Devender1 aDutta, Nilutpal1 aVinod, Chathakudath, P.1 aPeter, Sebastian, C. uhttps://library.ncl.res.in/content/dopant-and-exfoliation-induced-simultaneous-modification-charge-density-and-c%E2%80%95c-coupling