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Photocatalytic H 2 production from methanol is sustainable, yet challenges remain in avoiding carbon-containing gaseous by-products. Titanium silicalite-1 (TS-1) zeolite possesses attractive photocatalytic performance, but lack of modification strategies due to its microporous framework. Herein, we developed a pre-anchoring strategy to confine ultra-small Pt clusters inside TS-1 with ultra-low loading (0.2 mol%), in which Pt were anchored in Ti−OH nests by electronic metal-support interaction (EMSI). The optimal catalyst achieved a remarkable H 2 generation rate of 63.2 mmol g–1 h–1 in CH 3 OH solutions, along with the production of high-value chemical HCHO as the oxidation product with 96.9% selectivity. Investigations reveal that the EMSI between Pt and Ti facilitated the selective decomposition of CH 3 OH to H 2 and HCHO, leading to a nearly zero-carbon-emission process. Accordingly, we propose a light-driven carbon-negative "CO 2 →CH 3 OH→H 2 " route, coupling CO 2 utilization and green H 2 production with CH 3 OH as the intermediate, therefore offering a new perspective for "liquid sunshine". [Display omitted] • Pt clusters were successfully encapsulated inside TS-1 by a pre-anchoring method. • The optimal catalyst achieved a remarkable photocatalytic H 2 generation activity. • HCHO is the main oxidation product with nearly 100% selectivity. • The strong EMSI between Pt and Ti facilitated CH 3 OH decomposition to H 2 and HCHO. • A potential light-driven carbon-negative "CO 2 →CH 3 OH→H 2 " route was proposed. [ABSTRACT FROM AUTHOR]

Photothermal CO 2 oxidative dehydrogenation of propane (CO 2 -ODHP) is an environmentally friendly and sustainable route for propylene production and CO 2 utilization. In the present work, we developed a Pt-GaN/SrTiO 3 dual-functional catalyst to facilitate the reaction. The catalyst achieved propylene and CO yields of 1 mmol·g cat -1·h-1 and 1.2 mmol·g cat -1·h-1 under photothermal conditions at 320 °C, surpassing the performance of previously reported catalysts. Additionally, control experiments and in situ DRIFTS analyses corroborated that GaN and Pt were primarily responsible for the activation of C-H and C O bonds, respectively, and the photothermal route worked via a distinguished intermediate for CO 2 activation in contrast to the thermal route. DFT calculations supported the reaction route involving the coupling direct dehydrogenation of propane and reverse water-gas shift reaction. The present work shines a light on the design of photothermal catalysts with dual functions, particularly for the activation of CO 2 and light hydrocarbons. Additionally, it proposes a strategy to initiate high-temperature reactions at relatively lower temperatures. [Display omitted] • Pt-GaN/SrTiO 3 photothermally catalyzed CO 2 -ODHP for the first time. • GaN and Pt were primarily activations of C-H and C=O bonds respectively. • The DHP was driven by promoting the RWGS. • Different CO 2 intermediates were involved in thermal and photothermal reactions. [ABSTRACT FROM AUTHOR]

Bismuth (Bi)-based catalysts have attracted great attention in electrocatalytic CO 2 reduction into formate, but suffer from modest activity due to insufficient active sites and slow protonation process. Here, two-dimensional (2D) defect-rich Bi 2 S 3 nanosheets are first achieved through chemical vapor sulfurization of Bi 2 O 3 solids. It is found that the defects enable the stable immobilization of S heteroatoms into 2D Bi lattice. A combination of computational and experimental analyses reveal that S dopants can not only facilitate water dissociation to construct proton-rich surface, but also concentrate potassium cations to stabilize *OCHO intermediates. Further cooperating with defects, the *OCHO formation can be both kinetically and thermodynamically boosted. Remarkably, the constructed Bi 2 S 3 nanosheets exhibit a high formate Faradaic efficiency (>90%) over a wide potential window and a high intrinsic stability over 200 h. The excellent performance in flow cell as well as promising solar-driven CO 2 electrocatalysis further demonstrate the great potential for practical implementation. [Display omitted] • 2D defective Bi 2 S 3 nanosheets were achieved through chemical vapor sulfurization. • The defects enable the stable immobilization of S heteroatoms into 2D Bi lattice. • S dopants can construct proton-rich surface by facilitating water dissociation. • The constructed Bi 2 S 3 NSs show a high formate Faradaic efficiency and stability. [ABSTRACT FROM AUTHOR]

Selective catalytic reduction of NO x with ammonia (NH 3 -SCR) under the exposure of multiple poisons in fly ash remains a great challenging issue for environmental protection. Herein, the intelligently self-tunable defense effects of Ce(SO 4) 2 additive modification for the V 2 O 5 /CeO 2 catalyst with excellent resistance against K and Zn co-poisoning was originally illustrated. The Ce(SO 4) 2 additive could firstly act as an inhibitor to certainly restrain the electron transfer between V and Ce species to decrease the redox property, but the high NO x reduction efficiency of Ce(SO 4) 2 modified fresh catalyst could be maintained due to the enhancement of vanadium species polymerization and acidity. Unexpectedly, the Ce(SO 4) 2 additive would smartly translate to act as a promoter over the co-poisoned catalyst to effectively combine with poisons, thus releasing most active vanadium species to exhibit superior co-poisoning resistance to K and Zn. This work provides a novel self-tunable multi-poisoning-resistant strategy via acid additive modification for SCR catalysts. [Display omitted] • Ce(SO 4) 2 modified vanadia catalyst was obtained to fight K and Zn co-poisoning. • Ce(SO 4) 2 modification greatly improved NO x conversion and co-poisoning resistance. • Ce(SO 4) 2 was inhibitor to restrain electron transfer between active V and Ce sites. • Ce(SO 4) 2 translates to promoter to fix K and Zn poisons among poisoned catalysts. [ABSTRACT FROM AUTHOR]