The anode oxygen evolution reaction (OER) is knownt ol argely limit the efficiency of electrolyzerso wing to its sluggish kinetics.W hile crystalline metal oxides are promising as OER catalysts,t heir amorphous phases also show high activities.E fforts to produce amorphous metal oxides have progressed slowly, and how an amorphous structure benefits the catalytic performances remains elusive. Now the first scalable synthesis of amorphous NiFeMo oxide (up to 515 gi no ne batch) is presented with homogeneous elemental distribution via afacile supersaturated co-precipitation method. In contrast to its crystalline counterpart, amorphous NiFeMo oxide undergoes af aster surface self-reconstruction process during OER, forming am etal oxy(hydroxide) active layer with rich oxygen vacancies,leading to superior OER activity (280 mV overpotential at 10 mA cm À2 in 0.1m KOH). This opens up the potential of fast, facile,a nd scaleup production of amorphous metal oxides for high-performance OER catalysts.

The electrosynthesis of valuable multicarbon chemicals using carbon dioxide (CO 2 ) as a feedstock has substantially progressed recently but still faces considerable challenges. A major difficulty lines in the sluggish kinetics of forming carbon−carbon (C−C) bonds, especially in neutral media. We report here that oxide-derived copper crystals enclosed by six {100} and eight {111} facets can reduce CO 2 to multicarbon products with a high Faradaic efficiency of 74.9 ± 1.7% at a commercially relevant current density of 300 mA cm −2 in 1 M KHCO 3 (pH ∼ 8.4). By combining the experimental and computational studies, we uncovered that Cu(100)/Cu(111) interfaces offer a favorable local electronic structure that enhances *CO adsorption and lowers C−C coupling activation energy barriers, performing superior to Cu(100) and Cu(111) surfaces, respectively. On this catalyst, no obvious degradation was observed at 300 mA cm −2 over 50 h of continuous operation.

A considerable challenge in the conversion of carbon dioxide into useful fuels comes from the activation of CO2 to CO2.− or other intermediates, which often requires precious‐metal catalysts, high overpotentials, and/or electrolyte additives (e.g., ionic liquids). We report a microwave heating strategy for synthesizing a transition‐metal chalcogenide nanostructure that efficiently catalyzes CO2 electroreduction to carbon monoxide (CO). We found that the cadmium sulfide (CdS) nanoneedle arrays exhibit an unprecedented current density of 212 mA cm−2 with 95.5±4.0 % CO Faraday efficiency at −1.2 V versus a reversible hydrogen electrode (RHE; without iR correction). Experimental and computational studies show that the high‐curvature CdS nanostructured catalyst has a pronounced proximity effect which gives rise to large electric field enhancement, which can concentrate alkali‐metal cations resulting in the enhanced CO2 electroreduction efficiency.

Single‐atom catalysts (SACs) are witnessing rapid development due to their high activity and selectivity toward diverse reactions. However, it remains a grand challenge in the general synthesis of SACs, particularly featuring an identical chemical microenvironment and on the same support. Herein, a universal synthetic protocol is developed to immobilize SACs in metal–organic frameworks (MOFs). Significantly, by means of SnO2 as a mediator or adaptor, not only different single‐atom metal sites, such as Pt, Cu, and Ni, etc., can be installed, but also the MOF supports can be changed (for example, UiO‐66‐NH2, PCN‐222, and DUT‐67) to afford M1/SnO2/MOF architecture. Taking UiO‐66‐NH2 as a representative, the Pt1/SnO2/MOF exhibits approximately five times higher activity toward photocatalytic H2 production than the corresponding Pt nanoparticles (≈2.5 nm) stabilized by SnO2/UiO‐66‐NH2. Remarkably, despite featuring identical parameters in the chemical microenvironment and support in M1/SnO2/UiO‐66‐NH2, the Pt1 catalyst possesses a hydrogen evolution rate of 2167 µmol g–1 h–1, superior to the Cu1 and Ni1 counterparts, which is attributed to the differentiated hydrogen binding free energies, as supported by density‐functional theory (DFT) calculations. This is thought to be the first report on a universal approach toward the stabilization of SACs with identical chemical microenvironment on an identical support.

Many platinum group metal-free inorganic catalysts have demonstrated high intrinsic activity for diverse important electrode reactions, but their practical use often suffers from undesirable structural degradation and hence poor stability, especially in acidic media. We report here an alkali-heating synthesis to achieve phase-mixed cobalt diselenide material with nearly homogeneous distribution of cubic and orthorhombic phases. Using water electroreduction as a model reaction, we observe that the phase-mixed cobalt diselenide reaches the current density of 10 milliamperes per square centimeter at overpotential of mere 124 millivolts in acidic electrolyte. The catalyst shows no sign of deactivation after more than 400 h of continuous operation and the polarization curve is well retained after 50,000 potential cycles. Experimental and computational investigations uncover a boosted covalency between Co and Se atoms resulting from the phase mixture, which substantially enhances the lattice robustness and thereby the material stability. The findings provide promising design strategy for long-lived catalysts in acid through crystal phase engineering.

The anode oxygen evolution reaction (OER) is knownt ol argely limit the efficiency of electrolyzerso wing to its sluggish kinetics.W hile crystalline metal oxides are promising as OER catalysts,t heir amorphous phases also show high activities.E fforts to produce amorphous metal oxides have progressed slowly, and how an amorphous structure benefits the catalytic performances remains elusive. Now the first scalable synthesis of amorphous NiFeMo oxide (up to 515 gi no ne batch) is presented with homogeneous elemental distribution via afacile supersaturated co-precipitation method. In contrast to its crystalline counterpart, amorphous NiFeMo oxide undergoes af aster surface self-reconstruction process during OER, forming am etal oxy(hydroxide) active layer with rich oxygen vacancies,leading to superior OER activity (280 mV overpotential at 10 mA cm À2 in 0.1m KOH). This opens up the potential of fast, facile,a nd scaleup production of amorphous metal oxides for high-performance OER catalysts.

Electrosynthesis of hydrogen peroxide (H2O2) in the acidic environment could largely prevent its decomposition to water, but efficient catalysts that constitute entirely earth‐abundant elements are lacking. Here we report the experimental demonstration of narrowing the interlayer gap of metallic cobalt diselenide (CoSe2), which creates high‐performance catalyst to selectively drive two‐electron oxygen reduction toward H2O2 in an acidic electrolyte. The enhancement of the interlayer coupling between CoSe2 atomic layers offers a favorable surface electronic structure that weakens the critical *OOH adsorption, promoting the energetics for H2O2 production. Consequently, on the strongly coupled CoSe2 catalyst, we achieved Faradaic efficiency of 96.7 %, current density of 50.04 milliamperes per square centimeter, and product rate of 30.60 mg cm−2 h−1. Moreover, this catalyst shows no sign of degradation when operating at −63 milliamperes per square centimeter over 100 hours.

A considerable challenge in the conversion of carbon dioxide into useful fuels comes from the activation of CO2 to CO2.− or other intermediates, which often requires precious‐metal catalysts, high overpotentials, and/or electrolyte additives (e.g., ionic liquids). We report a microwave heating strategy for synthesizing a transition‐metal chalcogenide nanostructure that efficiently catalyzes CO2 electroreduction to carbon monoxide (CO). We found that the cadmium sulfide (CdS) nanoneedle arrays exhibit an unprecedented current density of 212 mA cm−2 with 95.5±4.0 % CO Faraday efficiency at −1.2 V versus a reversible hydrogen electrode (RHE; without iR correction). Experimental and computational studies show that the high‐curvature CdS nanostructured catalyst has a pronounced proximity effect which gives rise to large electric field enhancement, which can concentrate alkali‐metal cations resulting in the enhanced CO2 electroreduction efficiency.